Chemical vapor deposition (CVD) is generally considered an appropriate method to fabricate microdevices, thin films, and high-quality two-dimensional layers such as graphene, MoS2, and BN.Even though some aspects such as high cost and low yield rate need to improve before using this technique industrially, CVD is a fundamentally excellent method to fabricate thin film electrodes, especially when highquality graphene layers are needed.It is known that metallic iron is a common catalyst in growing graphene layers or carbon nanotubes due to the high carbon solubility under CVD conditions.However, it is still a challenge to form few-layer graphene (FLG) by CVD on the surface of a self-organized Fe2O3 NPL without the destruction of their well-defined nanostructures, and there has been no report on the CVD growth and energy storage applications of an FLG-coated heterogeneous Fe2O3/Fe3C NPL. Here, we report the growth of FLG on an Fe2O3 NPL, simultaneously forming a heterogeneous Fe2O3/Fe3C structure, by low temperature CVD (for the fabrication process, see the Experimental Section and Figure S1).