Three-dimensional CuS hierarchical crystals with high catalytic activity had been successfully fabricated using a facile solvothermal process, The CuS microparticles showed different flower-like morphology and good dispersion by optimizing reaction conditions. It was found that using N,N-dimethylformamide (DMF) as the solvent reagent in the proper temperature conditions was favorable for the growth of hierarchically structured CuS. The hexagonal flower-like CuS synthesized at 170℃ for 60 min displayed broad-spectrum photocatalytic properties under ultraviolet (UV) and visible irradiation. The as-prepared CuS crystals exhibited good performance to decolorize methylene blue (MB) solution under visible light irradiation. The total organic carbon (TOC) removal of rhodamine B (RhB) solution was nearly 60% after 5 h of the natural sunlight irradiation, and the property was stable after testing over four recycles, demonstrating a potential application in waster water treatment.