Harvesting mechanical energy through triboelectric nanogenerators (TENGs) for effectively purifying water, self‐powered wastewater treatment system presents a promising solution to address both energy and environmental crises. However, issues such as side‐discharge and wear, resulting from interfacial charge transfer, seriously hinder the output and durability of TENGs, and then reduce the efficiency of self‐powered wastewater treatment. Here, an interface charge regulation technique is introduced that simultaneously boosts both output performance and durability of TENG, enabling a greater efficiency in self‐powered wastewater treatment. The interface charge regulation method, suppressing side‐discharge around electrodes with an innovative insulator design as well as boosting charge density through secondary collection, fully utilizes surface charges for power output and results in minimum wear by reducing the interface electrostatic force. Surface charge density of 0.8 mC m−2 between the Ethyl tetrafluoro ethylene and copper (µ = 0.35), with a threefold enhancement under ambient conditions, and durability of 500 000 cycles (a 12.5‐fold enhancement) are achieved. Furthermore, the removal efficiency for proposed self‐powered sewage filter system is improved onefold, indicating the potential for sustainable and practical applications.