Transcranial alternating current stimulation (tACS) has been proposed to modulate neural activity through two primary mechanisms: entrainment and neuroplasticity. The current study aimed to probe both of these mechanisms in the context of the sensorimotor μ-rhythm using transcranial magnetic stimulation (TMS) and electroencephalography (EEG) to assess entrainment of corticospinal excitability (CSE) during stimulation (i.e., online) and immediately following stimulation, as well as neuroplastic aftereffects on CSE and μ EEG power. Thirteen participants received three sessions of stimulation. Each session consisted of 90 trials of μ-tACS tailored to each participant's individual μ frequency (IMF), with each trial consisting of 16 s of tACS followed by 8 s of rest (for a total of 24 min of tACS and 12 min of rest per session). Motor-evoked potentials (MEPs) were acquired at the start and end of the session (n = 41), and additional MEPs were acquired across the different phases of tACS at three epochs within each tACS trial (n = 90 for each epoch): early online, late online and offline echo. Resting EEG activity was recorded at the start, end and throughout the tACS session. The data were then pooled across the three sessions for each participant to maximise the MEP sample size per participant. We present preliminary evidence of CSE entrainment persisting immediately beyond tACS and have also replicated the plastic CSE facilitation observed in previous μ-tACS studies, thus supporting both entrainment and neuroplasticity as mechanisms by which tACS can modulate neural activity.