Free-standing, flexible, paper-like Fe2O3/graphene/carbon nanotubes (Fe2O3/GCNTs) ternary hybrid film with a three-dimensional hierarchical structure is synthesized through a simple filtration and a subsequent reduction process. The Fe2O3 particles are densely anchored onto the GCNTs conducting network, which serves as an ideal host for fast and efficient lithium storage. The layered GCNTs network not only withstands the huge stresses caused by Fe2O3 expansion/extraction but prevents the agglomeration of Fe2O3 upon continuous charging/discharging. The as-synthesized Fe2O3/GCNTs hybrid film is directly used as an anode for both half and full lithium-ion cells. Electrochemical measurement results indicate a high reversible capacity and a good rate capability can be realized on the hybrid when tested in half cell system. Furthermore, the prepared anode also shows favorable operation in full cell system comprising LiCoO2 cathode. These superior electrochemical performances of the hybrid film can be ascribed to the unique micro-structure, surface properties, and the strong synergistic effects among the individual component.