Background and Purpose— Many studies have attempted to bring to light the neural correlates of poststroke motor impairment, but few have used multimodal approach to explain it. The aim of this study was to elucidate neural structural and functional correlates of upper limb motor impairment by combining electrophysiological, anatomic, and functional neuroimaging data. Methods— Forty ischemic stroke patients (median [min–max] age: 63 [33–82] years, time poststroke: 3.5 [1.1–58] months) with unilateral upper limb weakness were included. The upper limb motor impairment was defined by a motor composite score. Simple linear analysis followed by multiple linear regression analysis were performed to identify which variables (corticospinal excitability, laterality indices within the primary motor cortex or corticospinal [CST], and corpus callosum tracts integrity) were the best explaining factors of upper limb motor impairment. Results— There was a significant correlation between the resting motor threshold ratio and CST damage ( r = −0.50 [95% CI, −0.70 to −0.22]; P <0.001) as well as the motor-evoked potentials amplitude ( r = −0.73 [95% CI, −0.85 to −0.54]; P <0.001). Only the resting motor threshold ratio was retained by the multiple regression model and explained half of the variance (49%; P <0.001) of the upper limb motor impairment after stroke. Conclusions— The implementation of quantitative neurophysiological measurements such as the resting motor threshold as a surrogate marker of impairment could be considered in neurorehabilitation trials.