(1) Background: The Go/NoGo task and color-word Stroop task were used to investigate the effect of applying different frequency bands of neural oscillations to the lDLPFC on inhibitory control modulation. (2) Methods: Participants were randomly categorized into four groups and received HD-tACS at 6, 10, and 20 Hz or sham stimulation at 1.5 mA for 20 min. All participants performed a color-word Stroop task and Go/NoGo task before and immediately after the stimulation; closed-eye resting-state EEG signals were acquired for 3 min before and after the tasks. (3) Results: There were no significant differences in the Go/NoGo behavioral indices task across the four groups. In the color-word Stroop task, the Stroop effect of response time was significantly reduced by 6 and 10 Hz stimulations compared to sham stimulation, and the Stroop effect of accuracy was significantly reduced by 10 Hz stimulation. There were no significant differences in the frequency range-specific (delta, theta, alpha, beta, or gamma) resting EEG power before and after stimulation. (4) Conclusions: HD-tACS at 6 and 10 Hz effectively improved participants’ performance on the color-word Stroop task, demonstrating the importance of the lDLPFC in interference inhibition and supporting a causal relationship between theta and alpha oscillations in interference inhibition.