Chirality has become an important research subject. The research areas associated with chirality are under substantial development. Meanwhile, graphene is a rapidly growing star material and has hard‐wired into diverse disciplines. Rational combination of graphene and chirality undoubtedly creates unprecedented functional materials and may also lead to great findings. This hypothesis has been clearly justified by the sizable number of studies. Unfortunately, there has not been any previous review paper summarizing the scattered studies and advancements on this topic so far. This overview paper attempts to review the progress made in chiral materials developed from graphene and their derivatives, with the hope of providing a systemic knowledge about the construction of chiral graphenes and chiral applications thereof. Recently emerging directions, existing challenges, and future perspectives are also presented. It is hoped this paper will arouse more interest and promote further faster progress in these significant research areas. Chiral graphene hybrid materials have emerged as a rising star in multidisciplinary fields with significant potentials. This review paper systematically summarizes the progress made in chiral graphene hybrid materials, with the hope to provide a systemic knowledge of the construction of chiral graphenes and their chiral applications. Recently emerging directions, existing challenges, and future perspectives are also presented. Chirality has been infiltrated into various research areas including chemistry, material, pharmaceutical, bioengineering, agriculture, environment, etc. Undoubtedly, chirality has become one of the foremost “elements” indispensable for human being to keep healthy and living normal life. For the development of science and technologies, design and exploration of powerful materials are one of the necessary prerequisite research themes. This is also true for chirality‐associated academic research and industry applications. Numerous chiral materials have been created and are still under active exploitation for uses in chiral separation, asymmetric catalysis, chiral recognition/sensing, and even chiral illuminant materials. Accordingly, combining chirality with advanced materials will surely lead to new materials with promising potential uses. This has been well exemplified by the successful integration of graphene family materials and chirality.Chirality is an essentially fundamental attribute of nature. Its implications have been well recognized in both fundamental research and industry, in particular from the disclosure of the course for the “thalidomide” tragedy.1 From Graphene and its analogues, primarily graphene oxide (GO), and reduced graphene oxide (RGO), currently still draw rapidly increasing attention of scientists from multidisciplines worldwide. Graphene has distinctive nanostructure and a variety of superior thermal, mechanical, and electrical properties. The fascinating structure and properties make graphene‐family materials hold large promise for potential applications in many areas including catalysis, sensors, electronic/photonic devices, inorganic/metallic nanocomposites, supercapacitors, energy storage, batteries, and biological and nanomedicine applications. Excellent review papers provide comprehensive overviews on graphene family materials from fundamental, structure, properties and applications. Aside from the special 2D nanostructure features and the corresponding thermal and conducting superiority, graphene also has high surface area . This additional attribute enables graphene to be an ideal candidate for developing materials toward separation/adsorption and as carriers for catalysts. GO retains the basic properties of graphene with sp2‐hybridized carbons on the aromatic network, but meanwhile contains sp3‐hybridized carbons bearing hydroxyl, carboxyl, and epoxide functional groups on the top and bottom surface and edges. The presence of the rich oxygen‐containing groups endows GO sheets with significant capability of further functionalization via covalent bonds and noncovalent interactions. Exploiting functionalized GO materials has become one of the most hot research topics especially in nanomedicine and bioengineering areas. The efforts have provided innumerable advanced functional materials, nearly having been hard‐wired into all science and technology fields. Among the numerous research directions concerning graphene‐derived functional materials, there is one intriguing research topic dealing with the connection of graphene with chirality, which is still filled up with various mystery even today.In the last decades, 2‐D materials began to gather wide interest due to their unique structures and huge potential applications. As a typical 2D material, graphene has attracted large attention since it was first reported in 2004.15 Gra chiral postfunctionalization using other chiral substances  constitutes the most popular way for developing chiral graphene materials. This is the case especially with GO. GO contains abundant oxygen‐containing active groups including hydroxyl, carboxyl, and epoxide groups. These reactive groups provide powerful and versatile “handles” to covalently graft achiral and chiral moieties onto graphene sheets. In addition, noncovalent interactions also can be taken to attach chiral moieties onto graphene sheets due to the 2D architecture and the oxygen‐containing functional moieties. The noncovalent interactions may be hydrophobic effect, π–π stacking interaction, electrostatic effect, and so on. Moreover, the specific 2D architecture of graphene sheets facilitates them to load a considerable amount of external substances, implementing highly efficient utilization of surface area since both sides and edges of each graphene sheet are all easily available.Chirality, as an intriguing natural phenomenon extensively existing in nearly all scaled structures, has been exploited in multitude areas, in particular chemistry, biochemistry, medicine and pharmacology. Graphene, as a rapidly rising star and typical 2D material, has exhibited huge potentials in diverse fields. If graphene family materials and chirality are rationally combined in one single entity, the resulting chiral materials are anticipated to demonstrate series of superior properties and find a number of uses. This consideration has been justified by the myriad reports in literature. So far graphene‐based chiral materials have advanced substantially and are still in rapid progress, owing to judiciously combining the advantages of graphene and those derived from chiral structures. Even though graphene can be awarded with structural chirality through special processes like twisted stacking and buckling,40 chi synthetic polymers, and natural macromolecules) to much more completed chiral substances consisting of metal elements and chiral organic components . Self‐assembly processes are also frequently used for constructing graphene‐containing functional chiral materials. Generally, these chiral hybrid materials were designed and explored with definitely intended applications, that is, as chiral catalysts, chiral separating media, chiral detectors , and in biomedical area. Striking advancements have been made; however, so far there has been no such a review paper to systemically summarize the scattered studies, most likely because of the multiple disciplines involved in a topic under discussion. To demonstrate the significant advancements and in particular to promote future progress, this comprehensive overview paper is prepared accordingly. It summarizes the state‐of‐the art studies focused on chiral graphene hybrid materials (CGHMs), as illustrated in Scheme Pristine graphene sheets tend to accumulate because of the hydrophobic skeleton, which is undesirable for graphene layers to retain a homogeneously dispersed state. Attachment of chiral components on graphene for chiral functionalization simultaneously helps to overcome this intractable trouble. Up to date, a great number of chiral sources have been taken to create graphene‐based chiral hybrid materials, from organic molecules  of amino acids play vital roles in human being health. If error occurs to these conditions, neurological disorders may appear like Parkinson's, Huntington's and Alzheimer's disease. Typical amino acids have at least one carboxyl group and one amino group. The reactive functional groups facilitate amino acids to readily undergo chemical reaction with GO. In addition, the polar moieties also render amino acids with capability of forming hydrogen bonds with the functional groups on GO sheets. Typically, Yin group used proline to chirally functionalize GO, with the aim to develop a hybrid chiral catalyst. A variety of materials have been taken as supports to immobilize proline and its derivatives. The supports can be polymers, inorganic materials like silica and magnetic nanoparticles, cyclodextrins, and ionic liquids. The layered structure and desirable properties of graphene enable it to be a new alternative for acting as supporting material for immobilizing proline. Characterizations demonstrate that l‐proline could be efficiently loaded on the two sides and edges of GO layers through hydrogen bonding and/or ionic interaction. The noncovalent interactions between proline with GO is illustratively shown in Figure  The resulting chiral hybrid was subsequently used as chiral catalyst for catalyzing direct aldol reaction. Considering the highly similar molecular structures of chiral amino acids, the work from Yin can serve as a versatile platform for using other amino acids for chiral functionalization of GO. Moreover, diverse amino acids are anticipated to give rise to chiral hybrids with individual properties and applications.The amino acids used to combine with graphene are summarized in d humans.63 Nowl‐phenylalanine and then combined the chiral product with graphene through noncovalent contacts. Herein pyrene moieties were selected to act as fluorophore. The as‐prepared chiral composite worked as chiral chemical sensors for enantioselective detection of natural acryclic monoterpenoid enantiomers, (R)‐(+)‐ and (S)‐(−)‐β‐citronellol. The chiral sensors show high sensitivity and selectivity. In view of the large number of amino acids and their potential chiral derivatives and the numerous fluorophores as well, innumerable chiral sensors and even other chiral materials and devices can be constructed based on similar building blocks, following the preparation strategy created in the study. Despite chiral detection has great potential to be applied in many areas, it currently still remains challenging in practice due to the substantial difficulty in discriminating enantiomers that possess the same chemical composition and nearly identical physical properties and differs only in steric conformation. The chemical sensors prepared through integrating a chiral moiety, a fluorophore, and graphene may provide straightforward and effective tools for chiral discrimination.Besides pristine amino acids, their derivatives alike also can be attached to graphene layers for diverse purposes. Kwak and co‐workers first chiral‐functionalized pyrene with Boc‐contacts.42 Herπ–π stacking, electrostatic interactions, etc.) for attachment of amino acids onto graphene, covalent bonds provide more choices and versatile approaches for the purpose of chiral functionalization of graphene. The abundant variety and number of reactive functional groups contained on GO sheets make covalent bonding between GO and amino acids highly feasible. Compared with noncovalent interactions, GO layers and amino acid moieties covalently bond together show higher stability. Making a full use of the carboxyl and epoxide groups on GO to respectively undergo amidation reaction (carboxyl groups) and epoxide ring‐opening reaction followed by amination reaction (epoxide groups) with the amino functionality on amino acids is a simple and popular approach to chiralizing GO. A typical illustration for preparing chiral hybrid materials is presented in Figure  Zhang et al. established another process for grafting amino acid onto GO. Making use of the hydroxyl and epoxide groups on GO sheets, carboxyl groups are introduced on GO first and then undergo esterification reaction with hydroxyl group in 4‐hydroxyl‐l‐proline. Taking the method, l‐proline was covalently anchored on GO. The graphene/l‐proline constructed chiral hybrids have proved to be good heterogeneous chiral catalyst especially for catalyzing direct asymmetric aldol reaction, as to be discussed in Section Apart from noncovalent approaches . In fact, apart from chiral proline, many studies have demonstrated that graphene is a robust catalyst support for immobilizing catalytically active organic molecules, the hybrid catalysts from which can catalyze a variety of reactions including oxidation reactions, Friedel–Crafts reactions, Aldol/Michael additions, epoxide ring‐opening reactions, one‐pot reactions, multicomponent reactions, and even polymerizations. The powerful catalytic capability of the resulting hybrid catalysts is attributed to the advantages of graphene, including large surface area, strong adsorption capacity, and high chemical stability. Easy attachment of catalytic moieties on graphene, in particular GO sheets, is another driving force for the research area to keep active. Additionally, graphene and the derivatives have a flat sheet‐like structure and a single layer of carbon atoms, thus providing a large open surface area that is readily accessible to reactants with low mass transfer resistance. Much more hybrid catalysts of the type, including both chiral and achiral ones based on graphene, are under intense development at present. Considering the milestone implications of catalysts in the development history of chemistry academia and chemical industry, the endeavors along the direction will as always maintain hot in the foreseeing future. The studies are expected to lead to far‐reaching impacts in both fundamental research and industrial events.Durmaz et al. took a different route to introduce proline onto GO, in which aminopropyltriethoxysilane (APTES) first reacted with GO, resulting in GO‐NH2.53 The The chiralized GO was characterized by circular dichroism (CD) and UV–vis absorption spectroscopy to elucidate its optical activity. For recording the spectra, the chiral GO was dispersed in deionized water and a homogeneous aqueous dispersion was obtained. The recorded CD and UV–vis absorption spectra are presented in Figure π–π conjugation of the C−C bonds in GO, whereas the latter reflects the n–π transition , the two absorption peaks were overlapped by that of cystine. However, they showed similar absorption to those of l‐ and d‐cysteine  complex and attachment of it onto GO sheets through the terminal amino groups in the complex; step‐2, reduction of GO with NaBH4; and step‐3, elimination of the copper ions to form the chiral nanocomposite hybrid. The built method is potentially usable for functionalization of other substrate materials aside from GO. Meanwhile, it is also potentially applicable to other amino acids and even other chiral molecules for attaching them on diverse substrates. The idea of introduction of metal complex may be taken to develop metal complex catalysts through selecting appropriate metal elements and suited chiral ligands. The work thus deserves much more attention from multiple aspects , and such endeavors may lead to new chiral materials and even more chiral phenomena that cannot be observed in usual chiral material systems. The as‐obtained chiral hybrids may be subsequently exploited as chiral nanocomposite sensors, biological imaging, supercapacitors, among many others.More other processes have been exploited to covalently bond amino acids to GO. Mo et al. developed a three‐step route to attach e hybrid.80 The2.1.2α‐, β‐, and γ‐cyclodextrins , constitute another prevalent category of chiral sources for chiral functionalization of both graphene and GO. Nonetheless, obviously different from amino acids, cyclodextrins are incorporated with graphene and the derivatives much more through noncovalent interactions rather than covalent bonding, probably because of the relatively more difficulties in accomplishing reactions between cyclodextrins and graphene. Another reason may lie in the fact that substitution of the initial —OH groups on cyclodextrins may exert influence on their enantioselectivity and the ability to form inclusion complex with guest compounds.Cyclodextrins, frequently used in the form of pectively81), c synthetic chemistry, adsorption and separation, food chemistry, and chiral recognition. Owing to the relatively more studies have been devoted to constructing cyclodextrin/graphene chiral material systems, the studies will be classified into two subgroups for a convenient discussion. The classification is performed according to whether cyclodextrins and graphene sheets are combined via noncovalent interactions or covalent interactions. The relevant studies are summarized in Table No matter how cyclodextrin units are attached onto graphene, the unique molecular architecture of cyclodextrins (hydrophobic cavity and hydrophilic exterior) together with chiral nature makes them quite interesting for developing chiral functional materials. Enantioselective effects come into play when a pair of enantiomers form inclusion complex with cyclodextrin units, in which only the enantiomer well matched with the cyclodextrin cavity in terms of stereostructure can efficiently form inclusion complex. In the course of forming inclusion complex, the chiral hydroxyl groups sited in the rim of the cyclodextrin holes serve as stereoselectors. Furthermore, cyclodextrins can encapsulate hydrophobic guest molecules and modify the latter ones’ water‐solubility. As a consequence, cyclodextrins have found a lot of practical applications in diverse industries like drug delivery and biomedical engineering,91 syn As presented in Figure  Then GO was combined with cyclodextrins  to acquire GO/x‐CD hybrids, which were subsequently subjected to reduction, yielding RGO/x‐CD. In the next step, the RGO hybrids were taken to modify glassy carbon electrode (GCE), producing RGO/x‐CD/GCE that acted as chiral sensor for electrochemically recognizing 3,4‐dihydroxy‐phenylalanine  enantiomers. Herein, RGO and cyclodextrin units were bonded via hydrogen bonds. According to electrochemical measurements, the RGO/γ‐CD nanohybrid was found to be able to enantioselectively recognize DOPA. The limit of detection value and sensitivity were respectively determined as 15.9 × 10−6m and 0.2525 µA µm−1 for d‐DOPA; for l‐DOPA, the values were 14.9 × 10−6m and 0.6894 µA µm−1 respectively. In addition, the authors measured the oxidation peak potentials of DOPA enantiomers by cyclodextrin/graphene nanohybrid through cyclic voltammetry (CV), square‐wave voltammetry (SWV), and chronoamperometry (CA) techniques. It demonstrated that only RGO/γ‐CD could trigger an obvious relative potential difference in redox peak. The experiment results clearly demonstrate the difference of α‐, β‐, and γ‐CDs in enantioselectivity is due to their ability to form inclusion complexes with guest analytes. The study lays a foundation for design and preparation of chiral hybrids potentially usable for other chiral sensing materials and chiral analytes. The developed graphene‐based chiral analysis system may be suitable for preparing chiral membranes for chiral separation, chiral films for enantioselective detection, and chiral absorbents for chiral capture. Moreover, the study also disclosed the difference among the three classes of cyclodextrins, i.e., α‐, β‐, and γ‐CDs. According to the size of the chiral analytes, a category of cyclodextrin is selected, whose cavity should have commensurate size with the analytes.Graphene layer can be used as a scaffolding surface for anchoring cyclodextrin units, and the chiral product thereof can be utilized for diverse chiral applications. Massive efforts have been focused on this research topic. Currently, chiral hybrids of the type are still under active research. Zor and co‐workers developed a process to prepare chiral graphene modified electrode with the aim of discriminating chiral enantiomers.82 As α‐, β‐, and γ‐CDs) are all large enough to allow DOPA molecules to enter and form inclusion complex, the guest molecules enter the cyclodextrins’ cavity in different position. More specifically, as for α‐ and β‐CDs, DOPA molecules penetrated into the cavities in vertical position, while in the case of γ‐CDs, DOPA molecules entered into the cavity in horizontal position. The difference in this entering position, i.e., DOPA molecules orientation, led to varied binding energy and binding constant values between cyclodextrin units and DOPA molecules. In addition, the chirality of γ‐cyclodextrin units contributed to the chiral recognition ability toward DOPA enantiomers. The work reflects the necessity of molecular simulation, which can provide some theoretical support for experimental results and even insights into experimental phenomena that are difficult to understand. This point will be stressed again in Section Molecular docking studies provide some inspiring information for elucidating the observed phenomena. Although the three sets of cyclodextrins  for electrochemically sensing moxifloxacin hydrochloride enantiomers; RGO/β‐CD/MB/GCE  for electrochemically sensing chiral carboxylic acids; RGO/β‐CD for electrically and optically sensing tryptophan enantiomers; RGO/PNP/β‐CD/CPE  for electrochemically sensing chiral clopidogrels; RGO/PTCA/β‐CD  for electrochemically recognizing chiral phenylalanine; RGO/ferrocene/β‐CD for electrochemically recognizing phenylalanine racemate. These studies evidently show the importance of electrochemical sensors for enantio‐differentiating chiral compounds, due to their merits particularly in easy and fast operation.Based on the chiral hybrids constructed by graphene and cyclodextrin, more other components can be introduced into this basic material combination for developing new advanced chiral materials. Fu et al. prepared chiral nanohybrids composed of three components, that is, ntiomers.86 Othβ‐CD chiral magnetic nanocomposites and used them as tunable stationary phase in open‐tubular capillary electrochromatography for the chiral separation of tryptophan enantiomers. In the aforementioned studies, GO and RGO were taken for constructing the chiral hybrids. In recent years, graphene quantum dots (GQDs) emerge as a new class of hot nanoarchitectures for developing advanced functional materials, which will be specifically introduced in a separate section later on.Besides the above chiral hybrids derived from graphene, cyclodextrins, and other components, which were designed and prepared for chiral sensing or recognition, there are other investigations for implementing diverse chiral applications. Qiu and co‐workers prepared GO/ntiomers.102 In As shown in Figure α,β, and γ‐CD) were added. The process finally led to RGO‐cyclodextrin chiral composites. Combined with glass carbon electrode technique, the chiral composites exhibited electrochemically enantioselective recognition ability toward tartaric acid racemate. Cyclic voltammetry tests show that among the three glass carbon electrodes modified respectively with α, β, or γ‐CD/RGO chiral composites, the one with β‐CD gave peak current with the best shape. This was explained by the more stable inclusion complex formed between β‐CD and the guest molecules. RGO without the attachment of cyclodextrin was taken as a control sample. It showed low chiral response, proving the roles of cyclodextrin units in the chiral discrimination. It is useful to point out that, theoretical simulation may help disclose the different performances observed in α, β, or γ‐CD units. Indeed, theoretical simulation has been intensely utilized to assist in understanding chiral processes and the relevant mechanisms, for example, in heterochiral to homochiral transition in crystallization, chiral recognition, and formation of enantioselective inclusion complex.Noncovalent interactions provide straightforward processes for anchoring cyclodextrin units on graphene layers. But the stability of the chiral hybrids may be not satisfying enough for uses under certain conditions, especially at relatively higher temperature and in polar solvents. The rigorous conditions are not desirable for noncovalent bonds to retain stable. For further improving the stability, covalent bonds provide viable means for attachment of chiral molecules on graphene. Cheng and co‐workers built a convenient approach for covalently bonding cyclodextrins onto graphene.88 As Figure  The produced chiral hybrids were composed of GO, Fe3O4 nanoparticles, poly(NIPAM‐co‐GMA) and β‐CD. The preparation of the target chiral hybrids can be divided into four major steps: 1) deposition of Fe3O4 nanoparticles on GO to fabricate magnetic GO (MGO); 2) grafting active sites for subsequently initiating free radical polymerization on MGO, thereby forming MGO@PDA‐Br; 3) surface‐initiating atom transfer radical polymerization (ATRP) of NIPAM and GMA monomers to generate MGO@PNG (poly(NIPAM‐co‐GMA)); 4) grafting β‐CD units along the copolymer chains via epoxide ring‐opening reaction to finally form the chiral hybrid, MGO@PNG‐CD. The chiral hybrid shows multiple advantages in that GO provides high specific surface area, Fe3O4 nanoparticles provide magneticity, PNG chains provide temperature sensitivity, and β‐CD units provide chiral selectivity through forming host–guest inclusion complex. Furthermore, after enantioselective adsorption of tryptophan enantiomers, easy isolation of the chiral hybrid from mixed solution can be realized simply by using external magnetic field. Owing to the pH‐sensitivity of PNG polymer chains, desorption can be implemented with much ease.To enhance the amount of cyclodextrins attached on GO sheets and simultaneously to prepare smart and pH‐sensitive chiral hybrids, Cheng and co‐workers created a distinctive route for grafting cyclodextrin units on GO, as presented in Figure 105 Th Aside from graphene and cyclodextrin, other material also can be combined with the hybrid for developing advanced functional architectures with multicomponents, hierarchical structures, and excellent comprehensive properties, e.g., chiral hybrids constructed by carbon nanotube, RGO, and β‐CD toward electrochemically recognition of phenylalanine enantiomers; electrochemical sensors containing 3D graphene layers and hydroxypropyl‐β‐cyclodextrin units for recognition of tryptophan enantiomers. In particular noticeably, the existence of magnetic nanoparticles facilitates the chiral hybrids to be easily restored for further recycling use. Otherwise, it is an intractable task to isolate the chiral hybrids after use. Accordingly, the preparation methodology dealing with introduction magnetic nanoparticles may be applied to the preparation of other chiral materials to be hopefully used as chiral catalysts, chiral adsorbents, chiral selectors, etc. Apart from the popularly used Fe3O4 nanoparticles, other ingredients possessing magnetic property also can be taken for constructing chiral hybrids with magneticity, e.g., Co, CoFe, and CoFe2O4 nanoparticles. These potential candidates offer much more opportunities for developing chiral materials with magneticity, which in turn brings advantages for the chiral hybrids, including easy isolation after use and conveniently recycling use. Compared with the analogues without magneticity, the magnetic chiral materials are superior in terms of actual use operations. This allows the magnetic chiral materials to be more competent from the viewpoint of practical uses.The above preparation strategy offers a versatile platform for designing and developing chiral nanohybrids derived from graphene, cyclodextrins, and stimuli‐responsive polymer chains.105 As and rhodamine B rendering fluorescence for the hybrid chiral materials. Following the design and preparation strategy, more other building blocks may be utilized to provide their functions. For example, chiral pH‐responsive polymers, chiral temperature‐sensitive polymers, and chiral dynamic covalent structures  can be combined with chiral graphene hybrids to enable them to show stimuli‐responsivity. The as‐obtained smart chiral hybrids are interesting for diverse chiral applications. These stimuli‐responsive chiral graphene materials might become an attractive research direction in near future.Regarding the multicomponent chiral materials analyzed above, the essential underlying design strategy relies in: Graphene sheets afford large surface area while cyclodextrin units offer host–guest enantioselective interactions toward chiral analytes; the other ingredients make their corresponding contribution. for instance, magnetic particles providing magneticity;105 an2.1.3Table Just like cyclodextrins and the derivatives, other chiral small organic molecules can be combined with graphene, GO, and RGO through covalent bonds and/or noncovalent interactions. In this section, the cases with noncovalent interactions are introduced first, followed by those involving the formation of covalent bonds between graphene or its derivatives and chiral organic molecules. The chiral small molecules used for chiral functionalization of graphene are summarized in  The chiral hybrid showed electrochemical enantiorecognition for mandelic acid enantiomers. Also for the purpose of electrochemical sensing, Kong et al. synthesized a chiral ionic liquid and applied it as an electrolyte to incorporate with GO sheets for preparing chiral hybrid. The chiral hybrid was subsequently used as chiral modifier to construct an electrochemical sensor based on GCE, which can enantioselectively distinguish several racemic enantiomers including tryptophan, mandelic acid, malic acid, and tyrosine enantiomers, according to the response of peak current resulting in different forms. Apart from being used as chiral modifiers for preparing electrochemical sensors, chirally functionalized graphene can be taken for other chiral applications. Du et al. used maltodextrin to modify GO and the chiral product was used as chiral stationary phase in open‐tubular capillary electrochromatography for chiral separation of six chiral drugs, i.e., nefopam, amlodipine, citalopram hydrobromide, econazole, ketoconazole, and cetirizine hydrochloride. Compared with the pristine silica capillary, the resolution outcomes using the silica capillary after chiral modification were markedly improved. In order to bioimage prostate cancer cells, Mirabello and co‐workers prepared GO/chiral naphthalenediimide chiral nanohybrids, which showed promising applications in biosensing and bioimaging fields. Cong and co‐workers modified RGO sheets with a chiral liquid crystalline surfactant through noncovalent interactions, more specifically, through π–π interactions occurring between RGO sheets and the surfactant molecules. This study significantly expands the candidates used as chiral modifiers for functionalizing graphene. More unprecedented properties and promising uses are anticipated from the unique chiral hybrids consisting of chiral liquid crystalline structures.Jabbari and co‐workers developed a chiral biosensor using betamethasone as chiral selector through multilayered electrochemical deposition of betamethasone, overoxidized polypyrrole, and graphene sheets.121 Th first prepared GO sheets bearing acyl chloride reactive functional groups, and then the GO derivative reacted with chiral NH2‐BINOLs forming amide structures naphthalen‐2‐ol). The chiral product was further treated with Ti(OiPr)4 (tetraisopropyl titanate) to generate GO‐BINOL‐Ti chiral complex catalyst, which displayed good reactivity (99%) and modest enantioselectivity (45% e.e.) in the asymmetric addition reaction of diethylzinc to aromatic aldehydes. Serov and co‐workers functionalized mesoporous 3D graphene with tetracyanoethylene oxide and (S)‐(+)‐2‐pyrrolidinemethanol. The chiral product was used as chiral stationary phase for chromatographic separation, demonstrating pharmaceutical grade chiral separation of model ibuprofen and thalidomide racemic mixtures. Li group modified graphene using R‐mandelic acid‐linked calix[4]arene, which showed highly sensitive chiral recognition toward amino propanol in serum. Wang et al. reported a graphene sponge used for hemostasis, in which the chiral graphene material was prepared by crosslinking graphene with diaminopropionic acid.It has been definitely shown that covalent bonds can be employed for chiral functionalization of graphene, as demonstrated in the cases using amino acids and cyclodextrins discussed above. Yan group126 fi All these studies clearly show that a great number of small organic molecules can be potentially used as chiral sources for chiral modification of graphene family materials, and the resulting chiral hybrids are worthy to be continuously exploited for diverse applications. The substantial number of studies also evidence the significant importance of chiral graphene materials. According to specific needs, suitable chiral sources in particular the natural “chiral pool” can be utilized to develop chiral hybrids via reasonable integration with graphene and the derivatives. The “chiral pool” affords numerous possibilities for design and exploitation of novel advanced functional chiral materials.In a very recent publication, de Oteyza and co‐workers succeeded in transferring axial molecular chirality through a sequence of on‐surface reactions to prochiral graphene nanoribbons.128 Al2.2 Among the commonly used biomacromolecules, polysaccharides are the most widely used category for functionalization of graphene. Amylose, cellulose and derivatives, chitosan, and even two or more polysaccharides in combination are widely used for constructing graphene‐based chiral materials. The natural biomacromolecules used for chiral functionalization of graphene and the corresponding chiral applications of the resulting chiral hybrids are presented in Table Natural biomacromolecules generally possess stable physicochemical properties, good biocompatibility and rich functional groups, which provide many opportunities for further modification and regulation of their properties.133 Am2.2.1 they first modified silica core by introducing amino groups on its surface. The amino groups subsequently underwent amidation reaction with the carboxyl groups on GO, followed by the reduction of GO with hydrazine to provide RGO@silica hybrid. Finally, a cellulose derivative, i.e., cellulose tris was coated on the RGO@silica hybrid. The major procedure is illustratively presented in Figure  The eventually obtained chiral composite was used as stationary phase in chiral HPLC. In this work, the cellulose derivative was physically coated on reduced GO sheets, in which the phenyl groups preintroduced around cellulose backbones are considered forming hydrophobic interaction and π–π stacking with graphene skeleton. Apart from cellulose, other widely commercialized polysaccharides, e.g., starch (in particular amylose), chitosan, alginate, and hyaluronic acid, also can be taken as alternatives for combining with graphene and its derivatives, since these natural polysaccharides can be easily modified with compounds containing phenyl moieties, and especially these polysaccharides are chiral and hydrophilic. Once integrated with graphene family materials, they not only render graphene with chirality, but also favorably assist graphene layers in keeping dispersion state. In other words, the biomacromolecules helpfully prevent graphene sheets from accumulation, due to the hydrophilicity and steric hindrance of biomacromolecules.In most cases, polysaccharides are attached onto graphene sheets by noncovalent interactions. Taking the work from Li et al. as example,135 th CNCs are also employed as chiral source for developing chiral hybrid particles and chiral stationary phase for chiral separation. Zhu et al. fabricated a chiral smectic structure assembled from graphene and CNCs. As illustratively shown in Figure  also offer insights into 1D materials like CNCs. It may also stimulate new ideas since, aside from CNCs derived from cellulose, other nano‐ and microarchitectures also can be employed in order to chirally functionalize graphene and to construct advanced functional materials. The nano‐ and microscaled architectures include starch‐based nanoparticles, chitin and chitosan‐based nanocrystals. Stimulated by the growing requirements for sustainable materials, these biomass‐based architectures provide a lot of opportunities for accomplishing the purposes.Cellulose nanocrystals (CNCs) have become one of the most vibrant research fields in particular in advanced functional materials. In chiral materials research area, CNCs have attracted much attention. They are predominantly used to fabricate chiral optical materials due to their ability to form liquid crystal structures.151 CN2.2.2 The resulting chip‐based chiral hybrid was used as enantioselective open‐tubular capillary electrochromatography (OT‐CEC). As schematically shown in Figure Apart from polysaccharides, proteins constitute the second largest group of biomacromolecules that have been frequently employed for preparing chiral hybrids via integrating with graphene family materials. The integration can be realized through noncovalent interactions and/or covalent bonds. Qiu lab first deposited polydopamine–graphene oxide (PDA/GO) on a poly(dimethylsiloxane) (PDMS) microfluidic chip, and then conjugated bovine serum albumin (BSA) on it.141 Th affinity capillary monoliths were first modified with GO and then used HAS or pepsin as chiral selectors for the purpose of chiral separation  to explore the influence of spacer arm on enantio‐separation effect. Amongst the resulting chiral material systems, HAS‐GO‐EDA system exhibited the best chiral recognition ability; the as‐prepared columns demonstrated satisfactory column‐to‐column, run‐to‐run, and interday repeatability. HAS‐GO‐EDA based column also showed higher chiral selectivity toward nine pairs of enantiomers , when compared with the column without modification by GO. The results indicate that the stacking between biomacromolecules, GO sheets, and the silica substrate exert remarkable influence on the enantio‐discernibility of the chiral product. The stacked architecture directly affects the interactions between the chiral selecting sites and the chiral analytes to be differentiated.In the above study, BSA was noncovalently immobilized on GO, taking advantage of the large surface area of GO sheets. Proteins can be also efficiently attached on substrates alternatively through chemical reactions. In the study from Li and co‐workers,142 af Such chiral materials may be exploited as chiral sponges used in some specific situations, such as capturing chiral contaminants from wastewater for restoring chiral compounds and simultaneously solving chiral pollution in environment. The chiral monolith also may be developed as supports for chiral catalysts, due to their high porosity which is favorable to solve the problem of mass transfer in routine catalytic reaction systems.GO‐functionalized affinity capillary monoliths have promising potential for chiral applications. Considering that proteins and chitosan have abundant amino groups, the route developed by Li and co‐workers may be applicable to these types of biomacromolecules and even chiral small molecules containing amino groups. Also notably, monolithic materials show advantages of easy preparation and high porosity.155 Su glassy carbon electrode modified with RGO and γ‐globulin was fabricated for enantioselective differentiation of mandelic acids; and acetylcholinesterase/GO based sensors were constructed for electrochemical chiral detection of chiral molecules (methamidophos). The studies using various proteins to combine with graphene for diverse chiral applications have paved a solid foundation for further exploiting chiral materials of the kind. These novel chiral hybrids show a wide range of actual application potentials toward multiple research areas and industries, like chiral separation, asymmetric catalysis, chiral sensing and recognition, chiral adsorption, etc.In other studies, HAS, GO and indium tin oxide (after modification with 3‐aminoproyltriethoxysilane) based electrochemical biosensor was developed for chiral discrimination of tryptophan;143 gl2.2.3 Nonetheless, the studies using DNA and other types of biomacromolecules, with the exception of polysaccharides and proteins, are still quite limited in both variety and number. Owing to their unique structures and properties, the kind of biomacromolecules like DNA may perform distinctive functions when combined with graphene, which cannot be achieved in polysaccharides and proteins, much less chiral small molecules. With DNA as representative, the double helix structure may allow DNA‐based chiral hybrids to exhibit some fascinating properties. Accordingly, using DNA and other biomacromolecules that have not been explored extensively so far to develop novel chiral hybrid materials is expected to bring unique opportunities for chirality associated research areas. In brief, natural biomacromolecules can make much more contribution than just serving as chiral source. Their rational conjugation with graphene is a research subject deserving much more attention. The studies might not only lead to series of novel chiral hybrid materials, but also possibly provide some new insights into the intriguing chiral stereo‐architectures formed in biomacromolecules, for instance, double helices of DNA and α‐helices and β‐sheets of proteins. The endeavors may also stimulate rapid advancements of artificial helical polymers, which are designed and developed by imitating the natural analogues, as to be investigated in the next section.Besides the widely explored polysaccharides and proteins as summarized above, some other biomacromolecules also have potentials to be exploited for developing chiral materials. For instance, DNA was adopted as a chiral selector and immobilized in graphene‐based substrate, for the purpose of enantioselectively electrochemical recognition of tryptophan.47 Non2.3 In spite of the numerous materials consisting of graphene and polymer already created so far, the chiral analogues are quite limited in both type and number. Muthusamy group first prepared a chiral diamine starting from l‐phenylalanine; the diamine underwent polymerization with 3,3’,4,4’‐benzophenone tetracarboxylic dianhydride by thermal imidization method, thereby forming a chiral polyimide. The polyimide was then blended with GO to form a chiral GO/polyimide nanocomposite, aiming at investigating the effects of GO on the thermal, electrical, and morphological properties of the polymer. GO was found to uniformly dispersed in the chiral polyimide matrix; the dispersed phase formed strong bonds with the polymer matrix due to GO grafted with polyimide. The existence of GO improved the glass transition temperature of the polyimide from 225 °C (pristine polyimide) up to 251 °C (polyimide in the nanocomposite). The as‐obtained nanocomposite showed remarkable improvement in thermal, electrical, and mechanical performance, which is considered being derived from the good interfacial bonding between the two phases and the excellent dispersion of GO in the polymer matrix. Especially noticeably, biological studies show that the chiral nanocomposite exhibited antimicrobial effects against Gram‐positive and Gram‐negative bacteria. The chiral nanocomposite deserves more exploration. The antimicrobial property, together with the intrinsic easy processing ability of polymers, renders the chiral nanocomposite with promising applications as biological materials. Generally speaking, polyimides have better thermal and mechanical properties than common polymers and so have found practical applications in aerospace, electrical industries, automobile industries, fuel cells, etc. Affording polyimides with chirality makes them more interesting and expands their applications to chiral areas. Combination with graphene further favorably improves their integral properties and considerably extends their potential applications.Up to date, a myriad of composite materials has been explored based on graphene and polymers. The composites have been investigated in a wide range of research areas and industries.162 Inα‐helical and β‐sheet structures in proteins, helical structures in polysaccharides, which are closely correlated with noncovalent interactions. The regular stereo‐architectures and conformational chirality of biomacromolecules play vital roles for organisms to keep normal functions and biological processes. To acquire deep understanding of the chiral biomacromolecules, scientists have synthesized a series of chiral helical polymers and helical architectures imitating the natural counterparts. The typical artificial chiral helical polymers include polyacetylenes, polyisocyanides, polycarbodiimides, polys, and others. If combing synthetic helical polymers with graphene, the resulting chiral hybrids may incorporate the respective advantages of chiral polymers and graphene materials. Chen and co‐workers integrated poly(l‐glutamic acid sodium) (PLGA) and GO to fabricate chiral membrane. The synthetic chiral polymers used for chiral functionalization of graphene are summarized in Table Natural biomacromolecules form uniform chain conformations, like double helix in DNA, ractions.150 Th Owing to the π–π interactions between pyrene groups and graphene skeleton, the polyacetylene chains can be immobilized on graphene layers. For the copolymers derived from acetylenic monomer bearing pyrene substituents and chiral acetylenic monomers, they formed helical structures with predominant one‐handed helicity and thus possessed optical activity. After combined with graphene, the chiral helical copolymers retained their predominant helicity and thereby afforded the graphene/polymer hybrid with optical activity. This study opens up a route for chiral functionalization of graphene with chiral helical substituted polyacetylenes. On the basis of the study, Deng group further established a one‐step process for preparing chiral hybrid composed of graphene and helical polyacetylene. The preparation strategy is illustratively presented in Figure Among the artificial chiral helical polymers, substituted polyacetylenes have been substantially investigated and may serve as representative. Deng group introduced aromatic pyrene moieties in the pendant chains around polyacetylene backbones and integrated the polymer with graphene.174 Ow Diverse strategies can be taken to induce the otherwise racemic helical polymer chains to form one homohelicity or one predominant helicity. These strategies include using chiral catalyst, chiral monomer‐achiral monomer copolymerization, chiral field, and chiral postinduction. In the study  underwent HSSP with l‐ascorbic acid (l‐AA) as chiral source. Indeed, l‐AA is widely used as reducing agent for the reduction of GO. In this work, l‐AA played double roles simultaneously, i.e., as reducing agent for the reduction of GO and as chiral source for performing HSSP of the achiral monomer. Chirality transfer from l‐AA to the polymer chains was realized via the boric acid group in the monomer and polymer side chains, which can form borate with l‐AA. This study is interesting since the preparation methodology may be applicable to other achiral monomers, from which chiral graphene hybrids are also anticipated. From the viewpoint of the chiral product, it is also attractive because of the advantages of optical activity and high porosity, respectively, derived from chiral helical polyacetylene and graphene.In Figure 185 Diy Figure ,arene was used to functionalize graphene, eventually resulting in a viable electrochemical sensor toward amino propanol enantiomers. The studies mentioned above indicate that apart from cyclodextrin, other chiral compounds with distinctive architectures can serve as new platforms for developing chiral material systems intended for chiral detection, for instance, calixarenes and crown ethers. Calixarenes and crown ethers with chiral moieties can form inclusion complex with guests having commensurate size. Endowment them with chirality will lead to new types of chiral structures. Just like cyclodextrins, the chiral derivatives from calixarenes and crown ethers provide distinguished chiral building blocks for developing chiral graphene hybrids. Compared with cyclodextrins, calixarenes and crown ethers show superiority in that they can be tailored in the size of their cavity, since these synthetic macrocyclic compounds can be controlled in size at the initial design stage, according to actual requirements. This is remarkably discernable from the natural analogues like cyclodextrins. The developed chiral materials from calixarenes and crown ethers are anticipated to show some unique functions and utilities that usual chiral materials cannot perform.Other chiral structures offer new routes for chiral detection. For example, ntiomers.55 The cellulose and derivatives, and chitosan; proteins and enzymes like human serum albumin (HAS),γ‐globulin, acetylcholinesterase, DNA; and even the mixture of two type of biomacromolecules, chitosan and sodium alginate. As a subgroup of starch, amylose is a natural linear polysaccharide consisting of d‐(+)‐glucose units linked by (1‐4)‐α‐glycosidic bonds. Amylose can form host–guest inclusion complex with guest substances and even with polymer chains, through hydrophobic interactions between the guests and the helical‐shaped cavity formed along amylose macromolecule chains. Amylose has been substantially used as chiral selectors in chiral chromatography. Compared with other biomacromolecules, e.g., proteins and DNA, amylose shows advantages due to the low cost, easy availability, convenient manipulation, etc. Qu and co‐workers developed a reusable amylose‐graphene chiral composite for sensitive and visual fluorescent sensing probe toward tryptophan enantiomers. Noticeably, the resulting probe exhibits highly specific selectivity for tryptophan enantiomers over the other species of the same kind, as illustrated in Figure Chiral hybrids derived from graphene and biomacromolecules also show chiral recognition ability, as the chiral small molecules do. The examined biomacromolecules include polysaccharides like amylose,134 cel‐tryptophan is an essential amino acid, while d‐isomer has been taken as a precursor to synthesize neurotransmitter serotonin and anticancer drugs. As a consequence, various graphene‐based chiral material systems have been created for chiral detection and separation of tryptophan enantiomers, as can be seen in Tables  carboxymethyl cellulose/RGO, chitosan/RGO, chitosan/sodium/graphene/carbon nanotube, human serum albumin/GO, and DNA/RGO.Herein, it is pointed out that er drugs.232 As circular dichroism spectroscopy, chiral light, cavity‐enhanced polarimeters, microwaves, etc.), chemosensors are attractive because of the advantages in rapid sensing ability, high sensitivity, ease of operation, small size, and the need for just a small bit of sample. The substantial studies already accomplished along this direction also evidently demonstrate the significant relevance of the development of chiral sensors.Compared with other chiral detection and separation techniques  because of its relative simplicity and high efficiency. In chiral HPLC, chiral selectors are frequently immobilized on the stationary phase. Despite the powerful capability of the chiral stationary phases (CSPs) already commercialized, new CSPs are still in high requirement owing to the rapidly increasing variety and number of new chiral compounds, especially chiral drugs and agricultural chemicals. New chiral compounds also need corresponding CSPs for highly efficient resolution effects.Common chiral resolution techniques include gas and liquid chromatography and capillary electrophoresis.239 Th With the advancements of graphene‐associated materials and techniques, this unique type of 2D material began to be hard‐wired in CSPs used in chiral HPLC. In the work published by Li et al., cellulose derivatives were physically coated on RGO@SiO2 to prepare CSPs. With nine pairs of enantiomers as analytes , the as‐fabricated chiral HPLC showed improved separation performance relative to the control column without RGO, which was attributed to the existence of additional retention interaction between RGO and analytes, such as hydrophobic effect, π–π stacking, and hydrogen bonding.The CSPs in HPLC are generally composed of silica support coated by a functional chiral layer, which can be derived from chiral small molecules  or chiral biomacromolecules .7 WithS)‐(+)‐pyrrolidinemethanol to form MOD3 , which were modified successively by tetracyanoethylene oxide (TCNEO) to form MOD1 and then , other chiral small molecules also can play the role of chiral selectors in the form of CSPs. Maltodextrin‐modified GO was coated on electrochromatographic capillary, on which chiral drugs including nefopam, amlodipine, citalopram hydrobromide, econazole, ketoconazole, and cetirizine hydrochloride were separated. Compared with the pristine column, the modified one significantly improved the enantiomeric separation of the six racemic drugs. Separation experiments showed that the concentration of chiral selector, concentration of GO, buffer pH, applied voltage, and concentration of buffer all exerted influence on separation process.The usage of GO/ntiomers.102 Si In CEC family, enantioselective open‐tubular CEC (OT‐CEC) provides a promising analytical separation technique due to simple column preparation, no bubble formation, and stable electroosmotic flow application. It has gained quickly increasing interest in recent years. Nonetheless, OT‐CEC has some shortcomings for its low‐phase ratio and sample capacity, which is due to the limited amount of stationary phase coating. The limitation restricts extending application of OT‐CEC in chromatographic separation. Fortunately, graphene offers opportunities for increasing the surface area toward coating and sample capacity. Meanwhile, biomacromolecules provide important chiral building blocks for developing chromatography techniques.Capillary electrochromatography (CEC) integrates the high efficiency of capillary electrophoresis and the high selectivity of liquid chromatography phases and hence has become another powerful technique for chiral separation in the last decade.240 In BSA was stably immobilized in the poly(dimethylsiloxane) (PDMS) microchannel, fabricating a protein‐type stationary phase. Further characterizations showed that the modified ones exhibited some merits like much better wettability and more stable electroosmotic mobility when compared with the native PDMS microchannels. Besides, less nonspecific adsorption was observed in the modified ones. Chiral resolution tests toward chiral tryptophan, threonine, and chiral dipeptide demonstrate that the chiral columns had high enantioselectivity. HAS and pepsin also can be selected for combining with GO, aiming at modifying affinity capillary monoliths for chiral separation uses. All the endeavors above provide new insights into design and construction of graphene‐based chiral selectors. Facing the quickly increasing demand for chiral compounds, the chiral composites and the resolution results based on graphene family materials will guide the follow‐up studies along the direction.Bovine serum albumin (BSA) was conjugated with polydopamine‐GO nanocomposites and the resultant chiral hybrid was used as stationary phase in OT‐CEC.141 BS Summarizing, graphene family materials offer a valuable and versatile platform for creating unprecedented chiral hybrids. In spite of the large number of studies dealing with graphene associated with chirality, there still exists a large room for further exploitation of graphene‐based chiral materials.The studies focused on using graphene and derivatives after chiral functionalization may show some limitations. For the chiral graphene materials modified through weakly attaching or adsorbing chiral molecules, the chiral materials may not keep stable enough in polar organic solvents or under rigorous conditions. To overcome the deficiency, recently emerging spike of interest in graphene may provide some conceptual clues, for example, by preparing mesoporous 3D graphene nanosheets to exploit CSPs with chemical stability and cost‐effectiveness.127 Su3.3.2 Graphene and the derivatives  provide promising candidates for developing separating materials. Prior to the popular use of graphene, chiral membranes are generally constructed by a nonselective porous support and a coating of optically active layer working as selective factor for recognizing and separating analytes. An intractable task for a most part of chiral membranes is that they are generally subjected to a trade‐off between permeability and selectivity. This academic challenge is hopefully circumvented using graphene and the derivatives. Chen and co‐workers covalently grafted l‐glutamic acid on GO and the thus‐acquired chiral hybrid was fabricated into membrane, separately using cellulose acetate and anodic aluminum oxide as support. The chiral membranes were examined for separating 3,4‐dihydroxy‐l‐phenylalanine racemic (l‐ and d‐DOPA), with an illustrative setup as presented in Figure  It is indicative that the nonselective interactions, although quite weak, exert large influence on the eventual separating results.Chiral membranes have been explored with a relatively long history.242 Grl‐glutamic acid modified GO (Glu‐GO) with a polypeptide, poly(l‐glutamic acid) (PLGA), to introduce more chiral selectors. More recently, the same group introduced a carboxyl‐terminated ionic liquid (IL‐COOH) as a spacer to GO, which was followed by amidation reaction using l‐glutamic acid to form the chiral hybrid (GO‐IL‐Glu). Hybrid chiral membranes were eventually produced and showed further enhanced separation properties. They exhibited superiority in enantioselectivity and 1–3 orders of magnitude higher in flux than traditional chiral membranes. Relative to the chiral membrane derived from l‐glutamic acid modified GO and Glu‐GO/PLGA, the three‐component membranes (derived from GO‐IL‐Glu) showed an increase of ≈40−80% in enantioselectivity and an increase of an order of magnitude in flux. The remarkable improvement relies in the ionic liquid, which not only works as spacer (favorably expanding the interlayer spacing of GO layers), but also functions as active sites to favorably improve the grafting amount of chiral selector, i.e., l‐Glu (helpfully enhancing enantioselectivity of the composite membrane). In other words, both the flux and selectivity were concurrently improved in this case. In a very recent work, the authors explored chiral separation mechanism through molecular dynamics simulation, using d‐alanine modified graphene as chiral membrane models and d‐ and l‐phenylalanine as chiral probes. This study provides guidance on development and application of chiral membranes for enantiomer separation.To further improve the properties of chiral GO‐derived membranes, Chen and co‐workers prepared composite chiral membranes by combining electors.46 Mor3.3.3 Compared with asymmetric synthesis and chromatographic separation approaches, enantioselective crystallization has advantages in simple operation and cost‐efficiency. The process of crystallization is still widely utilized especially in drug mass production. Substantial progress has been made in understanding the thermodynamic and kinetic fundamentals inducing enantioselective crystallization. However, sustaining research is still important for optimizing crystallization processes. This technique needs the use of chiral additives as chiral inducer for triggering a certain enantiomer to preferentially crystallize or inhibiting one enantiomer from crystallization from the racemate, whereby chiral separation is realized.Even though chromatography techniques have become the most popular approaches for practically separating racemates, enantioselective crystallization technique is still required at present for acquiring some enantiomers.245 Co Multiple characterizations confirmed the success in grafting chiral polymer on the substrate. Chiral helical polymer chains afford GO with optical activity. The as‐prepared chiral nanocomposite was explored as chiral additive to induce enantioselective crystallization with racemic alanine as model analyte. The induced crystals have an e.e. value of 76%, displaying the potential use of the chiral nanocomposite in chiral related research areas.Chiral graphene derivatives can serve as a special type of chiral inducers. Zhu and co‐workers reported a “grafting from” strategy for immobilizing chiral helical poly(phenyl isocyanide)s onto GO nanosheets.171 Mu and chiral polymer particles attached on GO sheets. Based on chiral helical polyacetylene and GO, chiral hybrid particles with diverse shapes and magnetism were also constructed. The chiral hybrids were used to induce enantioselective crystallization of alanine and phenylalanine enantiomeric racemates. Taking racemic alanine as example, after inducing crystallization by chiral additives, beautiful rod‐like crystals with regular morphology were generated, which were experimentally proved to be predominantly constructed by l‐alanine  are going to be under continuous advancements. More efforts will be necessarily devoted to developing chiral materials as CSPs and chiral selectors in these processes. From the viewpoint of basic mechanism, the approaches involve liquid‐solid interactions and solid‐liquid equilibria. Studies focused on the aspect of exploring fundamentals may lead to new inspiration for further optimization of the chiral materials. Graphene and the derivatives offer a valuable platform for future studies. In addition, a judicious combination of diverse processes, e.g., HPLC followed by enantioselective crystallization, is anticipated to result in the desired chiral separation outcome.The findings from Deng group182 an3.3.4 The endeavors certainly exert positive effects on other chiral separation approaches, even on asymmetric catalysis. Additionally, in chiral adsorption processes, desorption procedure is usually carried out for acquiring enantiomeric compounds or for recycling use of adsorbent for more cycles. Accordingly, from the view point of practical operation, chiral adsorption is different from the other chiral separation techniques as described above.In chiral separation processes with either chromatography techniques, chiral membrane or enantioselective crystallization, the underlying driving force for the isolation of the two enantiomers from each other lies in the preferentially enantioselective interaction between the chiral selector with one enantiomer in each pair of enantiomeric racemates. In chromatographical approaches, the chiral selector means the CSPs , and it means the porous membranes in chiral resolution using chiral membranes; while in enantioselective crystallization, the chiral additives or chiral seeds serve as the role of chiral selectors. Furthermore, all these chiral separation processes involve liquid‐solid phase interactions. Some materials in particular those with porous 3D architectures show enantioselective adsorption ability. If the adsorption capacity and selectivity are satisfying, simple adsorption may avoid the necessity for using other tedious and high‐cost separation processes in some cases. In addition, chiral adsorption is frequently associated with academic terms such as chiral surface/interface, chirality induction, chirality transfer, etc. As a consequence, some researchers are engaged in exploring chiral adsorption from diverse viewpoints.249 Thβ‐CD on GO sheets, which was used for efficient resolution of asparagine enantiomers . Chiral porous materials constructed by graphene and chiral substances can be used as adsorbent for chiral adsorption. Using chiral monolithic adsorbent composed of chiral helical polyacetylene and graphene sheets .87 Chi The adsorption capacity for l‐ and d‐phenylalanine was 33% and 15%, respectively; for l‐ and d‐dopamine, adsorption capacity was determined to be 48% and 17% respectively. In this work, the authors designed and prepared chiral helical polymer‐graphene hybrid based on a biomimetic concept. More specifically, the polymer chains chemically grafted on graphene sheets undergo reversible transition between dissolution state . The two reversibly transitional states vividly simulate jellyfish in “free‐swimming” and “preying” moments. When the polymer chains undergo the “preying” process, they behave as a chiral “predator” to “capture” one enantiomer in a pair of enantiomers. In the subsequent “free‐swimming” state, they “release” the captured guest molecules. The above processes result in chiral separation effects via the capture‐release two steps. The preparation strategy is worthy to be explored further in depth, as it provides a good example for building biomimetic architectures.In addition, the chiral helical polymer chains covalently grafted on GO sheets show enantioselective adsorption toward dopamine and phenylalanine racemates.179 Th Yu and co‐workers reported a chiral adsorbent consisting of magnetic GO and chiral MOF. The chiral composite was formed through encapsulating magnetic GO sheets by homochiral MOF, thus integrating the advantages of each component judiciously in one single material. Synergistic effects existed in the components, thereby enabling the chiral composite to show fast, simple, and enantioselective capture of chiral drug intermediates. Solid phase extraction tests indicate that the chiral adsorbent has remarkable selectivity toward 1,1ʹ‐bi‐2‐naphthol and 2,2ʹ’‐furoin racemates. The presence of magneticity renders the chiral adsorbent with the desirable recycling use feature. Yu et al. prepared magnetic GO‐MOF architecture, possessing both magnetic property and excellent enantioselective capture ability toward chiral drug intermediates  through solid phase extraction process. The chiral porous nanocomposites show high enantioselectivity with e.e. reaching up to 85% for 2,2ʹ‐furoin and 66% for benzoin. The capture process can be completed within 4 and 6 min, respectively. After simple washing with appropriate solvent, the chiral nanocomposite can be conveniently recovered for repeated uses. Even after six recycling use cycles, the chiral composite retains their performance without apparent loss. The work provides an interesting “prototype” in integrating 2D and porous framework for constructing advanced functional materials. As for 2D materials, besides graphene family, MXene is rising rapidly nowadays and may be used; meanwhile, COF can be used as porous ordered framework structures. These newly emerging materials, when combined with chirality, may open up innumerable functional materials with intriguing properties and chiral applications.Some recently emerging materials have been utilized for constructing porous chiral materials and demonstrated tremendous potentials for developing new chiral materials. Among the new‐star materials, metal organic frameworks (MOFs) have witnessed striking progress. Like graphene, MOFs have been exploited in various research areas. Their fascinating porosity and ordered architecture enable them to be ideal building blocks for constructing chiral materials as asymmetric catalysts and enantioselective separating materials.250 Yul‐arginine, glutamic acid, phenylalanine, and cysteine) on GO via amidation reaction, and the chiralized GO was then attached with magnetic component (Fe3O4) by chemical coprecipitation method. The chiral hybrids were used for magnetic separation of proteins. The authors found that the extraction capacity for proteins were dependent on the type of amino acid, pH of the solution, the absence or presence of electrolyte, extraction time and the protein concentration. Thanks to the presence of magnetic component, the chiral nanocomposite can be restored and reused with good outcome. Proteins are the important material basis for life and closely linked to various forms of biological processes and life activity. Furthermore, proteins are the direct manifestation of life phenomena, so the isolation, enrichment, and analysis of proteins is of great significance in biomedical areas and life science. Unfortunately, detection of proteins is still a big challenge as they are usually present in a complex sample matrix, causing intractable interference for analysis. As a consequence, sample clean‐up, separation, and enrichment become inevitable processes before further analysis of proteins. Using magnetic chiral materials to isolate proteins opens up a promising alternative for circumventing the troubles mentioned just above, for which the study from Liang and co‐workers may create a competent protocol.Apart from optical resolution, chiralized graphene can be utilized for other purposes. For example, Liang and co‐workers covalently grafted four types of amino acids . GO was coated on LPF/M to form chiral hybrid hydrogels (LPF/M‐GO) through coordination interactions and hydrogen bonds between LPF/M and GO. Chiral transcription from the chiral hydrogels to thioflavin T took place through a complexation process, from which LPF/M‐GO‐ThT was generated, as illustratively shown in Figure In a very recent publication, Feng et al.255 pr3.4 Biological imaging makes it possible to directly visualize the biological processes at cellular and even subcellular levels within live cells. Multifunctional biosensors have been developed and used to detect and image intracellular biomolecules. However, efficiently detecting intracellular chiral molecule still remains an academic challenge. To explore artificial receptors that simultaneously exhibit enantioselectivity and low toxicity in living cells, Li group utilized β‐CD to modify GO, from which a chiral sensor was developed. It showed excellent sensing capabilities toward d‐phenylalanine both in solution and in living cells . The study establishes an efficient nanoplatform for targeted delivery and controlled release of chiral drugs for biomedical applications. Enantioselective effects in chiral drug delivery has become one of the research themes in pharmaceutical community. Owing to the chiral nature of the frequently used carriers and/or excipients  and the special chiral environment inside human body, chiral drugs may undergo specific enantioselective interactions with the chiral carriers and human body. Therefore, exploration delivery profile of chiral drugs becomes a significant research subject, given the percentage of chiral drugs grows rapidly at present. The work from Shuang et al. reflects that chiral graphene materials may be exploited for developing chiral carriers applicable to releasing chiral drugs, since a number of studies have shown the potential uses of graphene family materials as biomaterials. The chiral components summarized in Section  further evidences the importance of chirality in biological and physiological processes.Graphene‐based chiral materials demonstrate other significant application potentials in biological and biomedical area. Some chiral materials of the kind have been found to possess antimicrobial effects163 an Wang et al. used 2,3‐diaminopropionic acid (DapA) to crosslink graphene sponge (DCGS) for hemostasis treatment . Moreover, the film showed high heat transportation efficiency, excellent mechanical strength, and electrical conductivity. The created chiral composite film has potential for developing high‐performance thermal management films. In particular worthy to be mentioned is the chiral helical architecture formed by rod‐like CNCs. This distinctive construction enables the chiral composite material to show the appealing properties and huge application potentials yet to be explored systemically.Chiral graphene materials may further find actual applications in photoelectric area. Even though the efforts along this research direction are still scarce yet, the application potentials of such chiral materials have been demonstrated. For example, Zhu et al. developed high‐performance thermal management materials for dissipating excessive heat both in plane and through plane, which is of large interest to maintain efficient operation and prolong electronic devices’ life. For this purpose, the authors constructed a graphene‐derived composite film through conjugation with chiral cellulose nanocrystals (CNCs).267 Ch but also as optical devices. Zhu et al. reported a chiral smectic architecture prepared through self‐assembly of graphene oxide sheets and CNCs nanorods. The material with chiral smectic possess potential applications as optical metamaterials in optical modulation and mechanochromic sensing devices. As far as graphene‐based chiral liquid crystal materials are concerned, Feng and co‐workers recently published an overview paper, which can be referred to for more information. More detailed optical applications of chiral liquid crystal materials derived from graphene are reviewed therein. Graphene‐derived hierarchical and chiral materials have demonstrated promising application prospects in the currently active research area of energy storage, as reported by Tao and co‐workers Despite the limited studies at present, the unique structures and properties of graphene derivatives and the significant importance of chiral architectures will facilitate the chiral composite materials to find a wide spectrum of actual applications. The new‐generation materials might exert far‐reaching effects in modern science, technology, and human daily life.Nowadays, some architectures with nano‐ and microdimensional and unique profiles are gathering quickly increased interest. As a typical 2D material, graphene and the analogs have demonstrated numerous application potentials, as summarized in this overview paper. If the 2D material is rationally combined with a 1D material, e.g., CNCs, fascinating findings are high anticipated from the resulting composite. Some endeavors have been made under this topic. The judicious incorporation of graphene and CNCs may provide advanced functional materials with promising applications not only as thermal management267 bu4Graphene based chiral hybrid materials are under rapid progress currently. In spite of the rich variety and myriad of such chiral materials already created so far, more new chiral hybrids of the kind are still under active development. Graphene constructed chiral materials with more complex architectures and more fascinating functions are continuously emerging. More other components are introduced in graphene material systems to fabricate chiral hybrids with distinctive properties and applications. The emerging chiral hybrids currently under intensive exploration have demonstrated their superiority in new structures, properties, and functions.4.1 Accordingly, GQDs have drawn rapidly growing attention from various research communities. In addition, their excellent photostability, biocompatibility, and small dimension enable them to exhibit tremendous application prospects in particular in biomedical applications, sensing, batteries, LEDs, and as surfactant for polymerization. Particularly, the properties of small size, large specific surface area, and abundant edge sites endow GQDs with superiority for electrochemical sensing. Consequently, some groups take GQDs for developing chiral electrochemical sensors. Unfortunately, pristine GQDs do not have chiral structure. To afford chirality to them, so far primarily two strategies have been developed, as to be analyzed below. The chiral materials derived from GQDs are summarized in Table Graphene quantum dots (GQDs) refer to graphene sheets generally smaller than 10 nm. They possess similar fundamental properties to graphene. Nonetheless, compared with usual graphene sheets, GQDs have unique quantum confinement and edge effect  and thus have some fascinating properties that general 2D graphene sheets do not have.270 Ac Maçoas and co‐workers, and Segawa and co‐workers The second one can be denoted as “postchiralization” method, typically exemplified by the study from Haino et al. In the two approaches, the second one has witnessed rapid advancements due to the relatively easy introduction of chiral moieties onto GQDs either through noncovalent interactions or covalent bonds. Kong et al. reported a method to combine cyclodextrins with GQDs by noncovalent interactions, as presented in Figure  In this study, GQDs were prepared by pyrolysis of citric acid. They were then incorporated with β‐CD via hydrogen bonds occurring between the oxygen‐containing groups on GQDs and the hydroxyl groups on β‐CD. The as‐obtained chiral hybrids of GQDs/β‐CD were negatively charged due to the ionization of carboxyl groups on GQDs. The chiral hybrid was subsequently electrodeposited onto GCE for implementing the objective of electrochemically recognition toward tryptophan (Trp) enantiomers. The recognition results are displayed in Figure β‐CD/l‐Trp generates a significantly higher peak current than GQDs/β‐CD/d‐Trp. The peak current ratio of the former to the latter one is calculated to be 2.1. The results indicate that β‐CD preferably complexes with l‐Trp enantiomer, owing to the favorability of hydrogen bonds formed between the secondary hydroxyl groups on β‐CD rims and the amino group of l‐Trp, when the indole group of Trp enantiomers inserts into the cavity of β‐CD units.Two strategies have been developed for constructing chiral GQDs. The first strategy is “bottom‐up” method, well exemplified by the studies from Martín et al.,38 Maç Zhao et al. prepared GQDs/β‐CD chiral hybrids for discrimination of tyrosine enantiomers. The aforementioned studies provide convenient techniques for fast detection of chiral enantiomers. The above chiral hybrids were constructed by GQDs/chiral small molecules via noncovalent interactions. In some other studies, the two major components, that is, GQDs and chiral substances, were connected through covalent bonds. Herranz and co‐workers prepared chiral GQDs successively by acidic exfoliation and oxidation of graphite, followed by dialysis and esterification with enantiomerically pure (R)‐ or (S)‐phenyl‐1‐propanol. The chiral GQDs formed supramolecular aggregates with pyrene molecules. More interestingly, chirality transfer occurred from the chiral GQDs to pyrene units. In the study from Violi and co‐workers, GQDs were prepared and then covalently attached with l‐ or d‐cysteine using the carboxylic groups on GQDs and the amino group on cysteine to undergo amidation reaction. With covalently grafted cysteine moieties, the edges of the chiralized GQDs became crowded and then helical buckling occurred. The helicity of the buckled structures is associated with the chirality of the preintroduced cysteine. UV–vis absorption spectrum of the pristine GQDs revels a peak around 228 nm. For the chiral GQDs, the UV–vis absorption peaks shifted to 265 nm. CD spectra show that the l‐ and d‐cysteine functionalized GQDs have CD effects with opposite signs. The chiroptical asymmetry parameter (g‐factor) of chiral GQDs at the range of 250−265 nm is equal to 1 × 10−4, comparable to that of many chiral organic compounds. Further experimental and modeling data indicate that 3D twisting occurred to the graphene layers. In vitro evaluation tests of the GQDs were accomplished against liver cells to explore their biocompatibility. It is demonstrated that the GQDs have low cytotoxicity and differentiation of cytotoxicity between GQDs stereoisomers. Biocompatibility of the chiral GQDs opens up new routes for developing chiral drug delivery vehicles and more selective phototherapies; the twisted electronic states may lead to polarization‐based optoelectronic devices and new types of chiral catalysts.In other reports, Kong et al. prepared GQDs/tartaric acid chiral hybrids for electrochemical recognition of Trp enantiomers.279 Zhβ‐CD and cellulose can enhance the enantioseparation performance of β‐CD and cellulose, referring to the work from Qiu and co‐workers According to the experimental and molecular simulation data, GQDs provide extra interactions such as hydrophobic, hydrogen bonding, and π–π interactions while the chiral selectors (β‐CD units and cellulose macromolecular chains) enantioselectively interact with analyte enantiomers. The synergistic effects help to enhance the chiral recognition ability of the GQDs‐modified chiral hybrids. In this study, cellulose was combined with GQDs via noncovalent interactions. Besides cellulose, GQDs also can be combined with other biomacromolecules (see below), resulting in advanced functional chiral materials. Striking progress has been made under the research direction.GQDs combined individually with o‐workers281 Ac Owing to the strong interaction between GQDs and chitosan, the resulting chiral composite film was regular and uniform, and then applied to electrochemical chiral recognition of Trp enantiomers. In the chiral discerning process, chitosan provided a chiral microenvironment, while GQDs further amplified the electrochemical signals and thereby improved the recognition efficiency. In other words, the desired synergistic effects occurred between chitosan and GQDs, offering the chiral recognition toward Trp enantiomers. The work extends the applications of GQDs to electrochemically chiral sensors. Electrochemical recognition toward Trp enantiomers was also realized using self‐assembled architectures consisting of four components: GQDs, diphenylalanine, chitosan, and CTAB (cetyltrimethylammonium bromide). The assembled products showed enantiomerically differentiating ability. GQDs can also be combined with biomacromolecules through covalent bonds. Kong et al. functionalized bovine serum albumin (BSA) with GQDs. The obtained chiral hybrid served as a sensing platform for chiral recognition of Trp enantiomers. To form the covalently bonding connection, amidation reaction between BSA and GQDs was implemented. The resulting chiral sensor exhibited good biomolecular homochirality in recognizing Trp isomers, in which the chiral hybrid showed higher affinity toward l‐Trp than the opposite d‐isomer.GQDs were combined with chitosan, from which a chiral composite film was fabricated. The film was prepared by successive eletrodeposition of GQDs and chitosan on the surface of a GCE.282 OwThe above studies focused on combination of GQDs and chiral small biomolecules and biomacromolecules in one single material clearly demonstrate that GQDs and the chiral components provide their individual advantages. Synergistic effects can be anticipated from the two building blocks. In view of the good biocompatibility of both the two components, the chiral hybrids have promising potential applications such as biosensors, nanomedicines, and nanocarriers for delivering drugs. The materials of the kind are under intensive exploitation currently, but have shown bright prospects acting as a new generation of biomaterials. Aside from the biocompatibility, the chirality also enables them to be highly qualified for bio‐applications. Such chiral biomaterials are anticipated to be further developed as a new generation of biomaterials, since the routine counterparts lack the characteristic feature of chirality.4.2A majority of graphene‐based chiral materials are constructed by attachment of external chiral components onto graphene sheets, as demonstrated in the above sections. It means that the chirality of such chiral materials is stemmed from the attached structures bearing configurational chirality , conformational chirality  or a hierarchal chiral structure . Obviously discernable from these studies, chirality of some graphene and the derivative materials comes from constructional chirality. At this point, it is important to remark that to distinguish from configurational chirality, conformational chirality, and hierarchal chirality as mentioned above, constructional chirality refers to the chiral graphene materials in which the chirality is originated in factors rather than chiral molecules, biomacromolecules, polymers, chiral metal complexes, and chiral liquid crystals. Instead, constructional chirality is closely associated with asymmetric stacking of graphene sheets, or wrinkles with asymmetric architectures. In brief, constructional chirality is not derived from chiral (macro)molecules and other external elements, but from graphene sheets themselves. Compared with the ones with chiral (macro)molecules as chiral source, graphene materials possessing constructional chirality exhibit distinct characteristics in both structure and properties, and probably also in their functions and applications. as illustratively shown in Figure θ and rotational polarity). The stacking procedure included two steps. In the first step, a single‐layer graphene film was grown with a uniform crystalline orientation over the entire film; In the second step, the film was cut into pieces which were subsequently stacked layer‐by‐layer with a controlled θ angle on the basis of the known crystalline orientation while rotating anticlockwise or clockwise to form left‐ or right‐handed films connected by a mirror plane . Since the graphene sheets were positioned layer‐by‐layer with precise control of the interlayer rotation and polarity, the eventually resulting film exhibited tunable chiral properties correlated with the packing of graphene sheets. The chirality of the assembled films was confirmed by CD spectra measurement  to form chiral atomically thin film devices. It also opens up new approaches for realization and adjustment of chiral properties showing diverse electrical and optical characteristics. The concept of chiral stacking approach built in this work allows the investigation of the coupling between structural chirality and the spin and valley degrees of freedom. In addition, the chiral stacking approach and the fundamental exploration of the materials’ chirality dependent properties may promote the development of circuits integrating multiple functions together, which may exhibit advanced electrical, optoelectronic and chemical sensing performances.Park et al. prepared chiral atomically thins films through a chiral stacking approach,286 ast Figure .[286 was realized via chiral stacking rather than using additional chiral source as done in general endeavors. The study presents a fundamental understanding of the construction of materials’ chirality depending on structural asymmetry instead of (macro)molecular configurational or conformational asymmetry. Together with other chiral materials whose chirality is alike derived from stereo‐constructional asymmetry rather than molecular level asymmetry, the chiral graphene materials created in the work demonstrate that chiral architectures consisting of left‐ and right‐handed counterparts linked by mirror symmetry are useful for developing advanced electrical and optoelectronic applications such as polarization optics and spintronics.Especially noticeably, the chirality of the graphene films286 wa The underlying driving forces for realizing the chiral self‐assemblies are vigorous stirring and the presence of a polymer. It has ever been reported that stirring can induce chirality in initially achiral molecules and even induce circularly polarized luminescence from achiral materials. These findings indicate that physical stirring not only induces chirality at (macro)molecular level, but also at much higher levels. The investigation opens up a facile and universal strategy for self‐assembly of various low‐dimensional structures  for fabricating hierarchical chiral nanoarchitectures, like chiral nanofibers and nanorings and even more complicated architectures. Apart from carbonaceous materials, more other materials with diverse compositions and dimensionalities such as magnetic nanoparticles, metal nanowires, semiconductor quantum dots and so on can be assembled into chiral multiscaled materials.In virtue of external physical forces, graphene‐based materials can be awarded with constructional chirality, making the use of additional chiral molecular moieties unnecessary. Zhang et al. reported an interesting approach for fabricating assembled chiral nanoarchitectures  in vigorously stirred polymer solutions. Such chiral nanoarchitectures can be derived not only from 2D graphene nanosheets, but also from other nanomaterials like nanowires and nanotubes.287 Thπ–π stacking, and hydrogen bonding between GO sheets and HA. Rippled GO‐HA layers were generated and further assembled to form macroscopic chirality, due to interlayer and interdomain distortion which led to a twisted conformation of the C=C double bonds. Briefly, in the assembly process, ripples were formed in single GO‐HA layers due to noncovalent interactions. Such wrinkled layers further assembled into higher level structures having twisted domains. The twisting structures rendered the ultimately generated materials with constructional chirality. There have been various strategies for producing polymeric materials with wrinkles at diverse scales. Polymeric materials may be wrinkled in bulk or have wrinkled surface through self‐assembly, interpenetrating polymer network, or under mechanical strain. Once coupled with chirality in the course of producing the wrinkles, a great number of hierarchically structured materials may be developed, which are expected to show macroscopic chirality because of their asymmetric hierarchical architectures.Wang and co‐workers developed a process for inducing chirality in GO based hybrid materials. GO and humic acid (HA) assembled into sandwich‐like complex which further assembled into twisted, long‐range‐ordered nanostructures via noncovalent interactions like electrostatic repulsive effects, le bonds.288 Br have a common point in that the chirality  was induced by special nanostructures  or twisting force (stirring) rather than by deliberately adding external chiral inducers. The preparation strategies are inspiring, might stimulating more new ideas for constructing chiral hybrids starting from graphene or GO. Theoretical studies indicate that graphene and the derivative sheets could have weak electronic chirality because of the existence of geometric distortion on the carbon hexagonal planar structure. Now it has been further demonstrated that rippled domains in 2D graphene sheets can be induced by external forces, thereby forming highly anisotropic geometry and generating constructional chirality at relatively macroscaled levels. Herein, it may be interesting to consider that if an additional chiral component is present in the process of producing wrinkles or twisted architecture, what would be the finally formed material? How about its micro‐ and macroscaled chirality? The as‐prepared materials, even though still at conceptual design stage, seem to be so highly fascinating that experimental exploration may be undertaken soon, from which unexpected findings are highly anticipated.The studies above288 ha4.33O4 nanoparticles) into the chiral hybrid derived from graphene, which endows the chiral hybrid with magneticity and further the ready restoration and recycling use thereof. The resulting magnetic chiral sensing system can specifically recognize histidine enantiomers. In another work, chitosan‐based molecularly imprinted polymers (MIPs)305 were integrated with RGO to subsequently modify glassy carbon electrode (GCE).306 Herein, S‐propranolol was taken as the template for producing MIP. The chiral sensors fabricated in this study demonstrated electrochemically enantioselective recognition toward chiral propranolol drugs . The endeavors provide some stimulations for further developing chiral hybrids based on graphene and even other organic and inorganic materials. MIPs, which have “lock‐key” features, when reasonably incorporated with graphene chiral materials, the as‐prepared chiral composite materials are expected to show a wide range of advantages, including high porosity, high selectivity, and optical activity as well. The high selectivity may enable the chiral materials to be qualified for actual uses and at the same time to be advantageous over the analogues. Such chiral materials bearing MIPs might find broad practical uses in sensing, separation, adsorption, catalysis, drug delivery, among other applications.Some special components are added in hybrids constructed from graphene and chiral moieties to afford distinctive properties that cannot be achieved in routine chiral graphene materials. One example is to combine magnetic ingredient  and 2D materials  provide a variety of candidates for developing chiral architectures of the kind. Their individual electronic, optical, mechanical properties and so forth may render the chiral composite materials with substantial uses.In the study from Zhu et al.,137 2D Nowadays the quest for effectively controlling and predicting the chirality of supramolecular artificial materials still keeps a highly active research topic, attracting the attention of scientists from diverse disciplines. The developed human‐made chiral building blocks and chiral supramolecular assemblies have proved to be of significant and wide applicability to a range of uses in detection and separation of chiral compounds and more other areas related to chirality. Based on graphene and helical silica nanotubes, Jung and co‐workers developed a type of chiral hybrid material through electrostatic assembly. The chiral hybrid integrates the electrochemical properties of graphene and enantioselective separation ability of helical silica. The authors realized the encapsulation of helical silica nanotubes with RGO sheets, providing a chiral hybrid material being capable of chiral transcription of organic substances attached on the surface. Thereby, the study demonstrates that chiral transcription can be implemented with the assistance of graphene sheet surface. Chiral transcription was also realized using GO sheets, as reported recently. The resulting chiral hybrids may be applicable to other chiral applications like chiral sensing and recognition, besides chiral separation. The studies above open up a new way for creating novel chiral functional materials by taking advantage of graphene and other components with distinctive architectures and properties.Chiral supramolecular architectures have witnessed substantial progress in recent years. The endeavors can favorably further our understanding of nature's ability to create functional materials that possess hierarchical structure over a wide range of size scale. Inspired by the hierarchical structures in nature, biomimetic architectures can be developed.305 No55.1It has been clearly demonstrated that numerous unprecedented chiral materials will be generated once graphene family materials are reasonably integrated with chirality feature. Indeed, the potential variety and number of such chiral materials are tremendous. Referring to the literatures and based on the studies from our owns, some challenges still exist at present, in spite of the striking advancements made in the construction and exploration of graphene‐based chiral materials. The challenges are stated as follows.1)Characterization of chirality. How to quantitatively determine the chiral structure and the corresponding optical activity of the chiral hybrids still remains a big academic challenge, since nearly all the hybrids are solid. Therefore, unlike the samples in solution state, in which the characterizations including CD spectra, optical activity and so on can be performed quantitatively. Although solid CD instrumentation has been put into practical use, the preparation of samples with controlled parameters is seldom an easy matter. That is, it is quite difficult to control all the samples for quantitative comparison, for instance, a uniform thickness of film samples, membranes, and coated/deposited layers and the regular size of particulate hybrids. In addition, the low transparence of the samples may also give rise to difficulty in precise characterization. In fact, at present nearly all the characterizations are qualitative or semi‐quantitative for chiral solid products. With the development of academic instruments, this issue may be satisfyingly solved in the near future.2)Enantiomeric excess values. For a most part of chiral applications ranging from asymmetric catalysis, chiral separation, to enantioselective detection, e.e. values provide more useful information regarding the chiral products derived from asymmetric catalysis reactions and the analytes of interest in chiral separation and enantioselective detection experiments. Unfortunately, in a majority of such experimentations, only few determined e.e. values. This situation may be associated with the difficulty in determining e.e. because of the challenges existing with instrumentation, as just mentioned above. Diverse instrumentations can be combined to measure e.e., for example, HPLC, CD, and optical rotation measurements may in combination assist in determining e.e. values. Moreover, the e.e. values reported in literature are not high enough. It indicates that there are still a large room for further improving the properties and functions of the chiral materials.3)Synergistic effects. To solve the issue just aforementioned in the above section, making a full use and further improvement of the synergistic effects between graphene and chiral components may be an effective way. For example, in our chiral adsorption tests, we found that graphene can contribute to enhancing the total adsorption capacity, but meanwhile it decreases the enantioselective during adsorption. This is easy to understand, since graphene sheets have large specific surface area and the architectures derived from graphene sheets are frequently porous. Accordingly, how to rationally take advantage of the individual merits of the major building blocks forming the chiral hybrid materials and simultaneously circumvent the limitations of each one still remains as a challenge. Further optimization of the composition, micro‐ and macrostructure and morphology of the chiral hybrids may be helpful to overcome the problems.5.2In spite of the existence of difficulties and challenges, rational combination of chirality with graphene family materials has become one of the most active research subjects. The studies along this direction have demonstrated widespread impacts on multitude areas including material, chemistry, pharmaceutical, agrochemical, biomedical, etc. Especially, the potential chiral materials of the kind and their applications seem to be unlimited. Nonetheless, some issues related to the development and exploration of chiral hybrids derived from graphene also deserve much more efforts. Future research directions, perspectives, and in particular the issues requiring more consideration may include:1) In other words, external chiral spices are no longer necessarily required. The as‐induced chirality, i.e., constructional chirality, has not been explored intensively yet. This type of chiral graphene materials is worthy to be investigated in depth, since they may show discernable properties and functions that cannot be observed in the analogues whose chirality is originated in additional chiral components. Additionally, GO sheets can form chiral liquid crystals and then assembled into macroscopic fibers with chirality. Graphene and its derivatives can possess luminescent behaviors by different manners . The luminescence property may be combined with chirality to further develop circularly polarized luminescence materials, another category of quickly developing materials. The potential applications of such a type of chiral graphene are still yet to be investigated. Graphene has been taken to develop metamaterials with distinguished electronic, optical, and magnetic properties. Their use potentials in solar‐thermal energy conversion, wave absorption, and electromagnetic shielding also cause a lot of interest. It is thus indicative that if graphene‐based metamaterials are combined with chirality, unprecedented materials with new phenomena and new utility may be highly anticipated. Graphene coupled with chirality provides huge opportunities for developing the newly emerging chiral metamaterials. For example, Masyukov et al. prepared terahertz chiral metamaterials with polarization manipulation ability, which is constructed by multilayered graphene. Hu et al. theoretically demonstrated that CD effects can be enhanced in chiral hybrid metamaterials composed of graphene and chiral metal nanocrystals at near‐infrared region. These studies indicate the bright prospects of chiral metamaterials developed from graphene.Constructional chirality and chiral metamaterials. Studies have demonstrated that graphene and the derivatives can be afforded with chirality through physical force driving the graphene sheets to twist and rumple in a single sheet or to stack in twisting.288 In2) On the other hand, chiral membranes have been manufactured via electrospinning process. It is hence hypothesized that chiral membranes based on graphene nanofibers may combine the merits of fibrous membranes and chirality. The as‐obtained chiral graphene derived nanofibrous membranes are expected to possess possible uses in chiral separation, chiral adsorption, chiral drug delivery, etc. In addition, nano‐ and microscaled chiral particles have been prepared using graphene nano‐ and microsheets. The chiral hybrid materials show enantioselectivity in chiral separation processes, e.g., in inducing enantioselective crystallization. Considering the advantages of nano‐ and microscaled architectures, graphene based chiral nano‐ and micromaterials are interesting both in nanofibrous and in particulate morphology.Nano‐/microscaled chiral materials. Graphene and the analogs have been fabricated into various chiral composites, and in turn assembled into hierarchical architectures. Graphene can be electrospun into nanofibers.320 On3) Through comparing simulation predictions and the corresponding experimental measurements, insights into further improvement of membrane properties were acquired. Molecular dynamics simulations, together with experimental studies, help researchers to well understand the support effects of graphene in the supported catalysts thereof. Schwerdtfeger et al. proposed a new concept for functionalization of graphene aimed at chiral separation. Computational simulations show that attaching suitable chiral moieties to the pore rim in graphene prevents the passage of the distomer, while letting the eutomer pass. Based on simulation results, the introduced chiral molecules play the role of a “gatekeeper.” Nonetheless, theoretical simulations are still seldom used. They sometimes provide useful information that experimental studies cannot provide. Moreover, they may offer some important guidelines for design and preparation of chiral hybrids starting from graphene family materials.Theoretical simulation. Experimental studies have made huge progress while theoretical simulations have been left far behind. Theoretical simulations may provide some guidelines for designing and preparing new chiral derivatives from graphene. For instance, molecular simulation has proved to be an effective tool to study graphene‐based membranes.323 Th4) Some studies show that graphene and the derivatives are toxic to living organisms. Here are some typical reports. Graphene exerts toxic effects on bacteria, mammalian fibroblasts; graphene oxide results in severe and persistent lung injuries. Consequently, graphene family may pose potential risks for human health and even for other biological organisms. To elucidate the issue, more studies are still required; in particular, more in vivo studies should be accomplished for the chiral graphene materials targeted for biological uses.Biological safety. One of the research directions concerning chiral graphene is to develop chiral composites intended for biological applications. Regarding the biological safety of graphene‐family materials, it is still under disputation.327 So5) The second one is related to colloidal substances. It has been shown that polymeric, metallic, inorganic, and complex nanoparticles have aggregated in atmospheric air and natural waters, resulting in the emergence of new contaminants and the associated adverse effects. As far as graphene is concerned, micro‐ and nanoscaled graphene may be gathered in nature, causing drastic impacts on ecology. This issue may be explored together with the first one to exactly make clear the effects of graphene family materials  on nature environment, including both human beings and other organisms. The third one is connected with chirality. Owing to the enantioselective effects of chiral species, the design, preparation, and use of chiral matters, especially chiral drugs, agrochemicals, food additives, and fragrances, all highlight one in a pair of chiral enantiomers. If this condition goes on, it will unavoidably lead to chiral species accumulation in nature; and eventually the original chiral equilibrium will be most likely destroyed. If so, catastrophic effects will occur to human beings and even the chiral nature. Accordingly, special attention should be paid to chiral graphene materials, from the beginning point of design, preparation, to use of them, and even the stage after use.Environmental concerns. Graphene‐related researches have grown at a spectacular pace in a wide range of disciplines. This situation has caused concerns about its health and ecosystem risks. Just like other materials derived from graphene, developing chiral graphene materials may lead to environmental pollution in three aspects presented below. The first one is associated with graphene. As typical 2D and advanced nanomaterials, the amount of graphene analogs increases rapidly each year, involving a large variety of scientific, engineering, technology, and material fields. The graphene family materials inevitably accumulate in environment and pose negative impacts on the environment and ecology systems.333 Th6) may be exquisitely designed and constructed to acquire advanced functionals materials like natural shells produced by biological organisms. The relevant studies clearly demonstrate the far‐reaching effects of chiralized graphene materials. This tendency will retain at least in the near future. The present review paper summarizes the explorations dealing with chiral graphene materials. The chiral species for chiralization of graphene family materials and their applications in the areas associated with chirality are systemically analyzed. Other relevant issues are also presented, including the newly emerging chiral graphene materials, the existing challenges, and the future perspectives. The continuing studies may not only lead to a great number of new chiral hybrid materials and accomplishment of practical applications, but also provide new insights into the homochirality of nature.Graphene has become one of the star materials due to its fascinating structure, properties, and functions. Meanwhile, chirality is the fundamental attribute of nature. A judicious combination of them, i.e., developing chiral graphene materials, has proved to be a valuable research subject. The efforts have led to innumerable new functional materials integrating the advantages of graphene and chiral materials. The as‐created chiral hybrid materials have demonstrated promising applications in nearly all the specific areas associated with chirality, including asymmetric catalysis, enantiodifferentiating detection, and enantioselective crystallization. Chiralized graphene is also developed for biological applications. More recently, chiral luminescent materials were developed based on graphene. Considering the ever‐growing importance of biomimetic materials, layered‐structure graphene sheets and chiral helical macromolecules  mThe authors declare no conflict of interest.