The corpus callosum (CC) is the major white matter tract connecting the left and right cerebral hemispheres. It has been hypothesized that individual variation in CC morphology is negatively associated with forebrain volume (FBV) and this accounts for variation in behavioral and brain asymmetries as well as sex differences. To test this hypothesis, CC surface area and thickness as well as FBV was quantified in 221 chimpanzees with known pedigrees. CC surface area, thickness and FBV were significantly heritable and phenotypically associated with each other; however, no significant genetic association was found between FBV, CC surface area and thickness. The CC surface area and thickness measures were also found to be significantly heritable in both chimpanzee cohorts as were phenotypic associations with variation in asymmetries in tool use skill, suggesting that these findings are reproducible. Finally, significant phenotypic and genetic associations were found between hand use skill and region-specific variation in CC surface area and thickness. These findings suggest that common genes may underlie individual differences in chimpanzee tool use skill and interhemispheric connectivity as manifest by variation in surface area and thickness within the anterior region of the CC.