PVDF/ZnO/CuS photocatalysts with ZnO/CuS heterojunctions were synthesized via electrospinning, hydrothermal, and ion-exchange techniques. As matrix materials, electrospun PVDF nanofibers are easy to be recycled and reused. ZnO nanorods anchored on PVDF nanofiber with high specific surface area provide abundant active reaction sites for photocatalysis. While the loaded CuS nanoparticles as a photosensitizer compensate the low quantum efficiency of ZnO and improve the visible-light photocatalytic efficiency. As a result, the PVDF/ZnO/CuS composited photocatalyst exhibits outstanding photocatalytic performance in exposure to UV and visible light owing to the suppressed recombination of electron-hole pairs and widened visible light absorption range. The kinetic constants of PVDF/ZnO/CuS nanocomposites under UV irradiation (9.01 × 10 min) and visible light (6.53 × 10 min) irradiation were 3.66 and 2.53 times higher than that of PVDF/ZnO (2.46 × 10 min & 2.58 × 10 min), respectively. Furthermore, PVDF/ZnO/CuS nanocomposites demonstrate excellent robustness in terms of recycling and reuse, which is advantageous in practical applications.