We studied the relationship between age-related differences in inter- and intra-hemispheric structural and functional connectivity in the bilateral motor network. Our focus was on the correlation between connectivity and declined motor performance in older adults. Structural and functional connectivity were estimated using diffusion weighted imaging and resting-state electro-encephalography, respectively. A total of 48 young and older healthy participants were measured. In addition, motor performances were assessed using bimanual coordination tasks. To pre-select regions-of-interest (ROIs), a neural model was adopted that accounts for intra-hemispheric functional connectivity between dorsal premotor area (PMd) and primary motor cortex (M1) and inter-hemispheric connections between left and right M1 (M1 and M1 ). Functional connectivity was determined via the weighted phase-lag index (wPLI) in the source-reconstructed beta activity during rest. We quantified structural connectivity using kurtosis anisotropy (KA) values of tracts derived from diffusion tensor-based fiber tractography between the aforementioned areas. In the group of older adults, wPLI values between M1 -M1 were negatively associated with the quality of bimanual motor performance. The additional association between wPLI values of PMd --M1 and PMd -M1 supports that functional connectivity with the left hemisphere mediated (bimanual) motor control in older adults. The correlational analysis between the selected structural and functional connections revealed a strong association between wPLI values in the left intra-hemispheric PMd -M1 pathway and KA values in M1 -M1 and PMd -M1 pathways in the group of older adults. This suggests that weaker structural connections in older adults correlate with stronger functional connectivity and, hence, poorer motor performance.