Understanding the neurocognitive mechanisms of the coordination of habitual and goal-directed behaviors is particularly important, as impaired coordination will cause various behavioral disorders. However, inducing habitual responses in human beings through repetitive stimuli-response training in a laboratory setting is a challenge. Well-trained sports experts, who have automatic perception-action associations towards expertise-related stimuli, provide a natural sample to address this critical knowledge gap. We used scalp electroencephalogram (EEG) to record the brain activity of well-trained sports experts when they performed a Simon task using expertise-related stimuli. By manipulating the congruency between the location of expertise-related stimuli and the response hand, we dissociated automatic habitual response and goal-directed inhibition control. We observed a stronger congruency effect on expertise-related stimuli than neutral stimuli. Particularly, sports experts exhibited larger response-locked lateralized readiness potentials (LRP) and stronger frontocentral beta band (15-25Hz) activity in the congruent condition than the incongruent condition, which indicate an enhanced automatic habitual response tendency towards expertise-related stimuli. In contrast, prominent mid-frontal theta (3-7Hz) activity observed in the incongruent condition signaled the involvement of inhibition control. Moreover, the response-locked lateralized readiness potential (LRP) amplitude and theta power showed significant behavioral relevance to performance efficiency. Taken together, these results suggest that sports experts exhibit an enhanced coordination process towards expertise-related stimuli, with automatic response preparation and proficient response inhibition through extensive training.