CuS nanoparticle/ZnO nanorod heterostructure arrays grown on carbon fibers (CuS/ZnO/CFs) were prepared successfully by a simple combination of a hydrothermal (HT) process and successive ionic layer adsorption and reaction (SILAR). The heterostructures of CuS/ZnO/CFs showed improved photocatalytic activity in the degradation of methylene blue (MB). Under visible light irradiation, the CuS/ZnO/CF heterostructures exhibited remarkable visible light photocatalytic activity, which was 7.1 and 8.0 times higher than those of ZnO/CFs and ZnO, respectively. Under simulated solar light irradiation, the photocatalytic activity of the CuS/ZnO/CF heterostructures was 1.4 and 2.2 times higher than those of ZnO/CFs and ZnO, respectively. The enhanced photocatalytic activity could be ascribed to the effective electron-hole separation and improved visible light utilization from the cooperative effect of the type II CuS/ZnO heterostructures and conductive CFs, as well as the efficient light harvesting and high surface area of the heterostructure arrays. Moreover, the CuS/ZnO/CF heterostructures can be easily separated and recycled with little loss in the photocatalytic activity due to their unique structural features.