The genus Caltha (Ranunculaceae) consists of 10 species of low-growing, perennial herbs distributed throughout the moist temperate and cold regions of both the Northern and Southern Hemispheres. Traditionally, the species have been divided into two sections: section Psychrophila in the Southern Hemisphere with diplophyllous leaves and section Caltha in the Northern Hemisphere with leaves lacking inflexed appendages. This study uses chloroplast and nuclear DNA sequences to determine the relationships among the 10 species, test the monophyly of sections Psychrophila and Caltha, trace the evolutionary history of diplophylly, and explore biogeographical hypotheses for the genus. Analysis of these data resulted in a well-resolved and well-supported phylogeny. Section Psychrophila (C. sagittata, C. appendiculata, C. dionaeifolia, C. obtusa, C. introloba, and C. novae-zelandiae) was resolved as monophyletic, indicating a single origin of diplophylly. The species of section Caltha (C. natans, C. scaposa, C. palustris, and C. leptosepala) formed a paraphyletic grade. The resulting phylogeny strongly supports a Northern Hemisphere origin for Caltha, followed by dispersal to the Southern Hemisphere (Gondwanaland). A vicariance model is invoked to explain present-day distributions in South America, Australia, and New Zealand.