We report a transparent and flexible polyimide (PI)-doped single-layer (PSL) phototransistor for the detection of visible light. The PSL was deposited on a SiO2 gate insulator by a co-sputtering process using amorphous indium-gallium-zinc oxide (IGZO) and PI targets simultaneously. The PSL acted as both a channel layer and a visible-light absorption layer. PI is one of the few flexible organic materials that can be fabricated into sputtering targets. Compared with the IGZO phototransistor without PI doping, the PSL phototransistor exhibited improved optoelectronic characteristics under illumination with 635 nm red light of 1 mW/mm2 intensity; the obtained photoresponsivity ranged from 15.00 to 575.00 A/W, the photosensitivity from 1.38 × 101 to 9.86 × 106, and the specific detectivity from 1.35 × 107 to 5.83 × 1011 Jones. These improvements are attributed to subgap states induced by the PI doping, which formed decomposed organic molecules, oxygen vacancies, and metal hydroxides. Furthermore, a flexible PSL phototransistor was fabricated and showed stable optoelectronic characteristics even after 10,000 bending tests.