High-definition transcranial direct current stimulation (HD-tDCS) is a potential neuromodulation apparatus for stroke rehabilitation. However, its modulatory effects in stroke subjects is still not well understood. In this paper, the offline modulatory effects of HD-tDCS on the ipsilesional primary motor cortex were investigated by performing wrist isometric contraction tasks before and after HD-tDCS in eleven unilateral chronic stroke subjects using a synchronized HD-tDCS and electroencephalogram/electromyography measurement system. This paper is a randomized, single blinded, and sham-controlled crossover study. Each subject randomly received three HD-tDCS (anode, cathode, and sham) with at least one-week washout period. Online feedback-guided medium-level wrist isometric contraction tasks were conducted for the affected upper limbs before stimulation and 10, 30, and 50 min after the end of 10-min 1-mA HD-tDCS. The characteristics of corticomuscular coherence (CMC), cortical oscillation power spectral density, and power spectral entropy were analyzed during tasks and compared across all sessions and stimulation conditions. Anode HD-tDCS induced significant CMC changes in stroke subjects, while cathode and sham stimulation did not induce significant CMC changes. The largest neuromodulation effects were observed at 10 min immediately after anodal HD-tDCS.