By employing an ultrasonic deposition followed by heat treatment, magnetite (Fe3O4)–graphene nanosheet (GN) hybrid anode was synthesized to examine its electrochemical performance in Li-ion battery. The Fe3O4 nanocrystals with an average size of 10nm can be homogeneously incorporated into the GNs to form Fe3O4–GN composites. In comparison with fresh GN anode, the composite anode exhibits high reversible capacity of 753mAh/g at 0.1C, high rate capability (533mAh/g at 5C), and enhanced cyclic performance with high coulombic efficiency. This improvement can be attributed to the fact that since Fe3O4 acts not only as a redox site but also as a spacer, the Fe3O4–GN hybrid creates a three-dimensional architecture that effectively facilitates ionic diffusion, Li-storage, and electronic transport. This result opens an efficient route for synthesis and application of GN hybrid as anode material for Li-ion batteries with superior performance.