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Currently, enhancing the output power of rotational‐mode triboelectric nanogenerators (TENGs) using various complicated systems is a contentious issue; however, this is a challenging process owing to the inherent characteristics of TENGs, namely, low output currents as opposed to high voltages. Thus, this study proposes a simple and innovative strategy for ultra‐high output peak power generation of TENGs called a self‐boosted rotational electrostatic‐discharge TENG (SRE‐TENG). The SRE‐TENG mechanism is unique as it is based on charge control and boosted discharge design, thereby achieving a remarkable peak power of 1103.8 W, peak power density of 140.6 Kw m−2, low optimum resistance of 100 Ω, and broad peak power generation range of 10 Ω to 1 GΩ. Diligent measurements and analyses of the peak and root‐mean‐square voltage and current outputs of the SRE‐TENG are conducted for various design variables and circuit configurations. The proposed SRE‐TENG mechanism is validated using experimental and multiphysics simulation results. The high‐output performance of the SRE‐TENG is demonstrated via the lighting of 3,000 LEDs and a 60‐W lamp array, continuous driving of a commercial sensor array, and hydrogen/oxygen generation via water electrolysis. [ABSTRACT FROM AUTHOR]