While studying at the William Esper Studio, her first acting job was as main role Destiny Evans in the only season of the web series reboot of the American soap opera One Life to Live (2013).
The role of Destiny was originated by actress Shenell Edmonds, who was offered the opportunity to reprise her role in the reboot but declined; Harrier took over the role after auditioning.
Her performance was generally praised with Errol Lewis from the Soap Opera Network saying she "[has] nicely taken on the life of [her character]" and "the chemistry between [her and her on-screen boyfriend] is instantly there while leaving you wanting more".

Harrier next guest starred as Amber in the television series Unforgettable (2014), and made her film debut in The Last Five Years (2014) as a young woman who has an affair with Jamie, Jeremy Jordan's character.
She was cast in the AMC pilot Galyntine (2014), opposite Alycia Debnam-Carey, which was filmed but was not picked up and never aired.
In 2015, she appeared in the film 4th Man Out , and in her last year at William Esper she was cast in Codes of Conduct, an HBO miniseries pilot created by Steve McQueen.
Harrier considers this pilot to be her "first real job".
The pilot was filmed but the series was canceled and never aired.

Harrier starred alongside Rowan Blanchard and Mahershala Ali in The Realest Real, a campaign film directed by Carrie Brownstein for luxury French fashion brand Kenzo in 2016.
She also modeled for various campaigns for brands including Calvin Klein and Louis Vuitton, and became an ambassador for the latter and luxury Italian jewelry brand Bulgari.

In 2016, she also booked the role of Peter Parker's love interest Liz in Spider-Man: Homecoming.
She did two auditions and then a screen test with Tom Holland before getting the role six weeks later.
Her character was loosely based on Liz Allan from the comics and Harrier was given the creative freedom to create a modern version of the character.
Released in 2017, Spider-Man: Homecoming was Harrier's major film debut and breakthrough, as well as a box office success, grossing over $880 million worldwide and receiving generally positive reviews.
While the film brought Harrier substantial fame and established her as an actress, her performance was met with mixed reviews with some critics praising her for avoiding the damsel in distress trope and breaking barriers as the first love interest of color, while others were disappointed in her character's development and lack of screen time.
Dana Schwartz of Marie Claire gave a negative review: "Liz is always reactionary; she doesn't do anything ... [she] could literally be replaced by an object and ... the movie wouldn't change at all."
Jim Vejvoda from IGN said "Harrier nicely plays against expectations".
Mark Hughes wrote for Forbes that Harrier is a "welcome change to the usual romantic interests in superhero film" and plays Liz as a "likable, sympathetic, type-A person".

In June 2017, it was announced that Harrier would be portraying Millie Montag in Fahrenheit 451, HBO's film adaptation of the 1953 novel of the same name, opposite Michael B. Jordan; however, her scenes were later removed by the director who decided the character did not fit with the storyline and wanted to shorten the film's runtime.
While studying at the William Esper Studio, her first acting job was as main role Destiny Evans in the only season of the web series reboot of the American soap opera One Life to Live (2013). The role of Destiny was originated by actress Shenell Edmonds, who was offered the opportunity to reprise her role in the reboot but declined; Harrier took over the role after auditioning. Her performance was generally praised with Errol Lewis from the Soap Opera Network saying she "[has] nicely taken on the life of [her character]" and "the chemistry between [her and her on-screen boyfriend] is instantly there while leaving you wanting more".
Harrier next guest starred as Amber in the television series Unforgettable (2014), and made her film debut in The Last Five Years (2014) as a young woman who has an affair with Jamie, Jeremy Jordan's character. She was cast in the AMC pilot Galyntine (2014), opposite Alycia Debnam-Carey, which was filmed but was not picked up and never aired. In 2015, she appeared in the film 4th Man Out , and in her last year at William Esper she was cast in Codes of Conduct, an HBO miniseries pilot created by Steve McQueen. Harrier considers this pilot to be her "first real job". The pilot was filmed but the series was canceled and never aired. 
Harrier starred alongside Rowan Blanchard and Mahershala Ali in The Realest Real, a campaign film directed by Carrie Brownstein for luxury French fashion brand Kenzo in 2016. She also modeled for various campaigns for brands including Calvin Klein and Louis Vuitton, and became an ambassador for the latter and luxury Italian jewelry brand Bulgari. 
In 2016, she also booked the role of Peter Parker's love interest Liz in Spider-Man: Homecoming. She did two auditions and then a screen test with Tom Holland before getting the role six weeks later. Her character was loosely based on Liz Allan from the comics and Harrier was given the creative freedom to create a modern version of the character. Released in 2017, Spider-Man: Homecoming was Harrier's major film debut and breakthrough, as well as a box office success, grossing over $880 million worldwide and receiving generally positive reviews. While the film brought Harrier substantial fame and established her as an actress, her performance was met with mixed reviews with some critics praising her for avoiding the damsel in distress trope and breaking barriers as the first love interest of color, while others were disappointed in her character's development and lack of screen time. Dana Schwartz of Marie Claire gave a negative review: "Liz is always reactionary; she doesn't do anything ... [she] could literally be replaced by an object and ... the movie wouldn't change at all." Jim Vejvoda from IGN said "Harrier nicely plays against expectations". Mark Hughes wrote for Forbes that Harrier is a "welcome change to the usual romantic interests in superhero film" and plays Liz as a "likable, sympathetic, type-A person".
In June 2017, it was announced that Harrier would be portraying Millie Montag in Fahrenheit 451, HBO's film adaptation of the 1953 novel of the same name, opposite Michael B. Jordan; however, her scenes were later removed by the director who decided the character did not fit with the storyline and wanted to shorten the film's runtime.
Laura Harrier