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Self-powered photodetectors are of significance for the development of low-energy-consumption and environment-friendly Internet of Things. The performance of semiconductor-based self-powered photodetectors is limited by the low quality of junctions. Here, a novel strategy was proposed for developing high-performance self-powered photodetectors with boosted electrostatic potential. The proposed self-powered ultraviolet (UV) photodetector consisted of an indium tin oxide and titanium dioxide (ITO/TiO₂) heterojunction and an electret film (poly tetra fluoroethylene, PTFE). The PTFE layer introduces a built-in electrostatic field to highly enhance the photovoltaic effect, and its high internal resistance greatly reduces the dark current, and thus remarkable performances were achieved. The self-powered UV photodetector with PTFE demonstrated an extremely high on–off ratio of 2.49 × 10⁵, a responsivity of 76.87 mA/W, a response rise time of 7.44 ms, and a decay time of 3.75 ms. Furthermore, the device exhibited exceptional stability from room temperature to 70 °C. Compared with the conventional ITO/TiO₂ heterojunction without the PTFE layer, the photoresponse of the detector improved by 442-fold, and the light–dark ratio was increased by 8.40 × 10⁵ times. In addition, the detector is simple, easy to fabricate, and low cost. Therefore, it can be used on a large scale. The electrostatic modulation effect is universal for various types of semiconductor junctions and is expected to inspire more innovative applications in optoelectronic and microelectronic devices.