We demonstrate a low-cost, simple-operation, and environmentally friendly magnetic grinding synthetic process to prepare nontoxic copper sulfide-based composites with photocatalytic activity. Using this efficient approach, CuS/ZnS and CuS/CdS composites were successfully synthesized from elemental powders without using any other additives or solvents. The formation of metal sulfides was confirmed using a series of characterizations. The photocatalytic activities of the as-prepared materials were evaluated by the degradation of methylene blue (MB), rhodamine B (RhB), and methyl orange (MO) dyes in the presence of hydrogen peroxide (H₂O₂), which served as an oxidant under visible irradiation. The degradation efficiencies of MB and RhB by CuS/ZnS and CuS/CdS composites were more than 95% in 30 min and the degradation efficiency of MO was more than 85% in 90 min. The photocatalytic activities of the CuS/ZnS and CuS/CdS composites were better than those of pure metal sulfides. In addition, the CuS/ZnS and CuS/CdS composites showed good stability toward photocatalytic degradation and their main reactive species for degrading organic dyes are photogenerated hydroxyl radical (˙OH). Reasonable photocatalytic reaction mechanisms are proposed to explain the photocatalytic processes of the CuS/ZnS and CuS/CdS composites.