AbstractGraphene and its composite hydrogels with interconnected three-dimensional (3D) structure have raised continuous attention in energy storage. Herein, we describe a simple hydrothermal strategy to synthesize 3D CoS/graphene composite hydrogel (CGH), which contains the reduction of GO sheets and anchoring of CoS nanoparticles on graphene sheets. The formed special 3D structure endows this composite with high electrochemical performance. Remarkably, the obtained 3D CGH exhibits high specific capacitance (C_s) of 564 F g⁻¹ at a current density of 1 A g⁻¹ (about 1.3 times higher than pure CoS), superior rate capability and high stability. It is worth mentioning that this methodology is readily adaptable to decorating CoS nanoparticles onto graphene sheets and may be extended to the preparation of other pseudocapacitive materials based on graphene hydrogels for electrochemical applications.