Cognitive control is the capacity to guide motor and perceptual systems towards abstract goals. High-frequency neural oscillations related to motor activity in the beta band (13−30 Hz) and to visual processing in the gamma band (>30 Hz) are known to be modulated by cognitive control signals. One proposed mechanism for cognitive control is via cross-frequency coupling whereby low frequency network oscillations in prefrontal cortex (delta from 2−3 Hz and theta from 4−8 Hz) guide the expression of motor-related activity in action planning and guide perception-related activity in memory access. However, there is no causal evidence for cross-frequency coupling in these dissociable components of cognitive control. To address this important gap in knowledge, we delivered cross-frequency transcranial alternating current stimulation (CF-tACS) during performance of a task that manipulated cognitive control demands along two dimensions: the abstraction of the rules of the task (nested levels of action selection) that increased delta-beta coupling and the number of rules (set-size held in memory) that increased theta-gamma coupling. As hypothesized, we found that CF-tACS increased the targeted phase-amplitude coupling and modulated task performance of the associated cognitive control component. These findings provide causal evidence that prefrontal cortex orchestrates different components of cognitive control via two different cross-frequency coupling modalities.