Recently, two-dimensional (2D) transition metal dichalcogenides, such as tungsten diselenide (WSe 2 ), have been intensively explored for numerous optoelectronic applications owing to their outstanding electrical and optical properties. Although previous reports have attempted to implement highperformance phototransistors based on WSe 2 through various organic molecule coatings, this method remains a key challenge since the surface charge transfer after the organic molecule coating may increase both ON and OFF currents of the device, severely limiting the signal-to-noise ratio (SNR). Here, we report a highly photosensitive WSe 2 phototransistor with electrically self-isolated C8-BTBT as the light absorption layer. The self-isolated C8-BTBT on the WSe 2 channel could act solely as a light absorption layer, without any electrical contribution into WSe 2 , resulting in a significant improvement in photosensitivity (i.e., SNR). The self-isolated C8-BTBT coating was found to improve the photosensitivity of the device by 1294% under UV light illumination (λ ex = 406 nm) with an incident light power density (P inc ) of 6.66 mW cm −2 . Our study confirmed that this electrical self-isolation technique for the light absorption layer can be effectively used for high-performance 2D photosensing applications.