Three-dimensional self-organized nanoporous thin films integrated into a heterogeneous Fe2O3/Fe3C-graphene structure were fabricated using chemical vapor deposition. Fewlayer graphene coated on the nanoporous thin film was used as a conductive passivation layer, and Fe3C was introduced to improve capacity retention and stability of the nanoporous layer. A possible interfacial lithium storage effect was anticipated to provide additional charge storage in the electrode. These nanoporous layers, when used as an anode in lithium-ion batteries, deliver greatly enhanced cyclability and rate capacity compared with pristine Fe2O3: a specific capacity of356 μAh cm2μm1(3560 mAh cm3 or ∼1118 mAh g1) obtained at a discharge current densityof 50 μA cm2 (∼0.17 C) with 88% retention after 100 cycles and 165 μAh cm2 μm1 (1650 mAh cm3 or ∼518 mAh g1) obtained at a discharge current density of 1000 μA cm2 (∼6.6 C) for 1000 cycles were achieved. Meanwhile anenergy density of 294 μWh cm2μm1(2.94 Wh cm3 or ∼924Wh kg1) and power density of 584 μW cm2μm1(5.84 W cm3or ∼1834 W kg1) were also obtained, which may make these thin film anodes promising as a power supply for micro- or even nanosized portable electronic devices.