Abstract Graphene-based three-dimensional hierarchical architecture is one of the most desirable templates to modify the electrochemical performance of the cathode or anode material with low conductivity for lithium-ion batteries (LIBs). Herein, three-dimensional VS4/reduced graphene oxide (3DVG) hierarchical architecture with VS4 particles homogenously wrapped by the graphene nanosheets has been synthesized via a facile one-pot hydrothermal process. The 3DVG composite anode demonstrates excellent electrochemical performance: it exhibits a large specific capacity of 1044.2 mAh g−1 (close to its theoretical capacity of 1196 mAh g−1) and remains 890.8 mAh g−1 after 80 cycles at 0.2 A g−1; it also has a large rate capacity of 479.2 mAh g−1 even at 4 A g−1. This superior performance of the 3D composite for LIBs is attributed to the porous 3D architecture with the conductive graphene interconnected network to guarantee the high conductivity and enable fast electron transport between graphene and VS4. Moreover, the 3DVG provides a hierarchical template to accommodate the volume change of VS4 particles during the electrochemical cycling. The 3DVG was proved as a high capacity anode material for LIBs.