Graphene sponge (GS) has been widely employed for water purification, but adsorption capacity loss frequently occurs during the formation of spongy structure. In this study, we reported the hydrothermal preparation of S-doped GS for the removal of Cu2+ with a huge adsorption capacity of 228 mg/g, 40 times higher than that of active carbon. The adsorption isotherm could be well fitted into the Freundlich model with a K-F value of 36.309 (L/mg)(1/n). The equilibrium adsorption could be fully achieved in the first 5 min. In the thermodynamics study, the negative Delta G indicated that the adsorption was spontaneous and physisorption in nature. The positive Delta H implied that the adsorption was endothermic. The changes of both pH and ionic strength had no apparent influence on the adsorption. S-doped GS could be easily regenerated by washing with acidic thiourea. Moreover, S-doped GS could be used for the adsorption of other heavy metal ions, too. The implication to the applications of S-doped GS in water treatment is discussed. (C) 2015 Elsevier B.V. All rights reserved.