Single‐atom nanozymes (SAzymes) are considered as the most promising candidates for natural enzymes due to their atomically dispersed active sites that closely resemble the metal active centers of their natural counterparts. However, a significant challenge still exists for improving their catalytic activities, retarding their practical applications. Herein, this article presents that through the application of a human self‐driven triboelectric device to impose electrical stimulus, the multiple enzyme‐like activities of a single‐atom copper nanozyme (Cu‐NC) are remarkably improved, thereby boosting cancer cell oxidative damage and death for realizing improved therapy. Under an electrical stimulus with 20 V voltage, the peroxidase, catalase, oxidase, and glutathione oxidase like activities of Cu‐NC are all improved to boost the catalytic generation of free radicals. Through calculation, this work analyzes how the electrical stimulus modulates the catalytic activity via decreasing adsorption energy of H2O2 on Cu active sites, increasing Cu dxy orbital near the Fermi level, and shifting the d‐band center of Cu, facilitating the catalytic reactions. This work opens new perspectives on improving single‐atom nanoenzymes for cancer therapy.