A novel visible-light flower-like CuS/graphene aerogels (CuS/GAs) photocatalyst has been synthesized via two-step solvothermal method. The CuS/GAs show outstanding synergies of adsorption and photocatalysis for anionic–cationic dyes degradation, which is attributed to unique network structure and excellent photoelectric properties of GAs. The high degradation ratio of Methyl orange and Methylene blue by synergy are 92% and 99.36%, which are about 4.1 and 3.2 times of that for pure CuS. The flower-like CuS/graphene aerogels resolve the low adsorption saturation problem of GAs and improve the photocatalytic performance of CuS, indicating CuS/GAs could be a promising photocatalyst for wastewater treatment.