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Ultra-flexible fibrous supercapacitors have been fabricated with oxidized carbon nanotubes grown on carbon fiber (OCNTF)/polypyrrole (PPY) brush-like electrodes, for the first time. Hierarchically mesoporous OCNTF serves as a large surface area-bearing electrically conductive substrate for the electropolymerization of PPY during the synthesis of OCNTF/PPY nanocomposites. Here, carbon fiber serves as a mechanical support for the OCNTF/PPY nanocomposite architecture and current collector for the supercapacitor. X-ray photoelectron spectroscopic analysis has revealed the presence of various oxygen-containing functional groups on the surface of OCNTF. The OCNTF/PPY supercapacitor exhibits a maximum gravimetric capacitance of 305 F g−1 with a gravimetric energy density of 42 W h kg−1 and a maximum volume specific capacitance of 14 950 mF cm−3 at a current density of 2.5 mA cm−2. The …