Studies suggested a relationship between frontal brain activity asymmetry and self-regulation; however, these measures are regarded as indirect despite their relevance, and the underlying brain mechanisms are still unknown. Our preregistered study investigated the link between frontal alpha asymmetry as a potential neuromarker of self-regulation and behavioral and brain activity components of inhibitory control. We utilized a randomized controlled sham-feedback design involving 65 individuals (46 females). Prior to and following non-invasive brain stimulation, resting-state EEG data were collected to assess frontal alpha asymmetry scores, and participants completed a stop signal task, including neutral and reward conditions. During transcranial direct current stimulation, a 2 mA current was administered with the anode placed on the right frontal site and the cathode on the left frontal site. Results showed no effect of the intervention on frontal alpha asymmetry or any of the behavioral or neural indices related to inhibitory control. However, event-related potential analyses showed that inhibitory brain activity in the reward condition correlates with resting-state asymmetry of frontal brain activity, indexed by frontal alpha asymmetry. Specifically, higher right relative to left frontal brain activity was associated with lower early-onset inhibitory activity, presumably originating from the inferior Frontal Gyrus, but correlated with higher late onset inhibitory control, presumably originating from the superior Frontal Gyrus. The results suggest a functional dissociation regarding the lateralization of frontal brain activity and early and late onset inhibitory brain activity.