Children with unilateral spastic cerebral palsy (USCP) have shown impaired bimanual coordination. The corpus callosum (CC) connects the two hemispheres and is critical for tasks that require inter-hemisphere communication. The relationship between the functional bimanual coordination impairments and structural integrity of the CC is unclear. We hypothesized that better integrity of the CC would relate to better bimanual coordination performance during a kinematic bimanual drawer-opening task. Thirty-nine children with USCP (Age: 6–17 years old; MACS levels: I-III) participated in the study. Measurement of the CC integrity was performed using diffusion tensor imaging. The CC was measured as a whole and was also divided into three regions: genu, midbody, and splenium. Fractional anisotropy, axial diffusivity (AD), radial diffusivity, mean diffusivity, number of voxels, and number of streamlines were evaluated in whole and within each region of the CC. 3-D kinematic analyses of bimanual coordination were also assessed while children performed the bimanual task. There were negative correlations between bimanual coordination measures of total movement time and AD of whole CC (p = 0.037), number of streamlines and voxels of splenium (p = 0.038, 0.032, respectively); goal synchronization and AD of whole CC (p = 0.04), and number of streamlines and voxels of splenium (p = 0.001, 0.01, respectively). The current results highlight the possible connection between the integrity of the CC, especially between the splenium region and temporal bimanual coordination performance for children with USCP.