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Hierarchical composites (CFP–PANI) of carbon fiber papers (CFP) and polyaniline (PANI) have been facilely prepared by in-situ polymerization of aniline monomers on the surface of CFP films, which were simply obtained by low-cost carbonization of widely used filter paper. The wood–celluloses, which serve as the main component and the backbone of filter paper, are key raw materials for fabricating energy-related devices. Carbon fibers with porous structure were formed after the cellulose fibers were carbonized at high temperature. And cross-linked conductive networks have been achieved with the carbon fibers connected with each other. Different amounts of aniline monomer were in-situ polymerized on the surface of CFP, resulting in the formation of three-dimensional (3D) free-standing composite paper of CFP–PANI. Compared with pristine CFP and pure PANI, greatly enhanced electrochemical performance of CFP–PANI composite has been successfully achieved, including high specific capacitance (334 F g −1 ), good cycling stability as well as excellent rate capability. These superior electrochemical properties of CFP–PANI composite paper can be ascribed to the hierarchical structure of CFP, strong interaction between CFP and PANI, as well as the synergistic capacitance performance of CFP films and PANI nanoparticles, suggesting CFP–PANI composite paper thus simply prepared is good candidate for applications in high performance energy storage fields. [ABSTRACT FROM AUTHOR]