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Freestanding and flexible graphene/polyaniline composite paper was prepared by an in situ anodic electropolymerization of polyaniline film on graphene paper. This graphene-based composite paper electrode, consisting of graphene/polyaniline composite sheets as building blocks, shows a favorable tensile strength of 12.6 MPa and a stable large electrochemical capacitance (233 F g(-1) and 135 F cm(-3) for gravimetric and volumetric capacitances), which outperforms many other currently available carbon-based flexible electrodes and is hence particularly promising for flexible supercapacitors.