Bimanual actions involve coordinated motion but often rely on the movements performed with each hand to be different. Older adults exhibit differentially greater variability for bimanual actions in which each hand has an independent movement goal. Such actions rely on interhemispheric communication via the corpus callosum, including both facilitatory and inhibitory interactions. Here, we investigated whether age differences in callosal structure and interhemispheric function contribute to this selective movement difficulty. Participants performed 3 force production tasks: 1) unimanual, 2) bimanual simultaneous, and 3) bimanual independent. Older adults had significantly greater interhemispheric facilitation during voluntary muscle activation. We also report a fundamental shift with age in the relationship between callosal tract microstructural integrity and interhemispheric inhibition (IHI). Specifically, older adults with relatively greater callosal tract microstructural integrity have less IHI. Furthermore, greater IHI was related to poorer bimanual performance (assessed by dominant hand force variability) in older adults on all tasks, whereas this relationship was only observed in young adults for the bimanual independent condition. These findings indicate changes in interhemispheric communication with advancing age such that older adults may rely on bilateral cortical cooperation to a greater extent than young adults for manual actions.