Graphene-based three-dimensional (3D) aerogel hybrids have recently emerged as a new class of functional materials and applied in many fields. In this work, we assemble the spherical CdS nanoparticles in situ in graphene aerogel (GA) by a facile one-pot hydrothermal method. The resultant CdS-GA hybrids possess a hierarchical porous structure and there is strong electronic interaction between CdS and GA, which enhances the adsorption capacity and photocatalytic activity for the elimination of organic contaminants in water under visible light irradiation, such as rhodamine B (RhB), methylene blue (MB), add chrome blue K (AcbK), methyl orange (MO), and ciprofloxacin (CIP). The removal efficiencies of CdS-GA for MO, MB, CIP, RhB, AcbK are 15.6, 6.6, 4.4, 2.8, and 22 times of pure CdS, respectively. Meanwhile, the resultant CdS-GA hybrids display good reusability. In addition, a photocatalytic mechanism is also discussed. This provides a valuable alternative to explore semiconductor-GA hybrids with outstanding adsorption capacity and superior visible-light induced photocatalytic activity. (C) 2019 Elsevier B.V. All rights reserved.