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This letter reports the fabrication and electrochemical properties of electrospun carbon nanofibers surface-grafted with vapor-grown carbon nanotubes (CNTs) as hierarchical electrodes for supercapacitors. The specific capacitance of the fabricated electrodes was measured up to 185 F/g at the low discharge current density of 625 mA/g; a decrease of 38% was detected at the high discharge current density of 2.5 A/g. The morphology and microstructure of the electrodes were examined by electron microscopy, and the unique connectivity of the hybrid nanomaterials was responsible for the high specific capacitance and low intrinsic contact electric resistance of the hierarchical electrodes. [ABSTRACT FROM AUTHOR]