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Transcranial direct current stimulation (tDCS) is a non-invasive stimulation method that can induce transient polarity-specific neuroplastic changes in cortical excitability lasting up to 1 h post-stimulation. While excitability changes with stimulation over the primary motor cortex have been well documented, the functional effects of stimulation over premotor regions are less well understood. In the present experiment, we tested how cathodal and anodal tDCS applied over the region of the supplementary motor area (SMA) affected preparation and initiation of a voluntary movement. Participants performed a simple reaction time (RT) task requiring a targeted wrist-extension in response to a go-signal. In 20% of RT trials a startling acoustic stimulus (SAS) was presented 500 ms prior to the “go” signal in order to probe the state of motor preparation. Following the application of cathodal, anodal, or sham tDCS (separate days) over SMA for 10 min, participants performed blocks of RT trials at 10 min intervals. While sham stimulation did not affect RT or incidence of early release by the SAS, cathodal tDCS led to a significant slowing of RT that peaked 10 min after the end of stimulation and was associated with a marked decrease in the incidence of movement release by the SAS. In contrast, anodal tDCS resulted in faster RTs, but the incidence of release was unchanged. These results are consistent with the SMA playing a role in the pre-planning of movements and that modulating its activity with tDCS can lead to polarity-specific changes in motor behavior.