Graphite felts modified with atmospheric pressure plasma jets (APPJs) are applied as electrodes in an all-vanadium redox flow battery (VRFB). APPJ flow penetrates deeply into the graphite felt, improving significantly the wettability of the graphite felt inside out and, thereby, enhancing graphite fiber-electrolyte contact during battery operation. The energy efficiency of a VRFB was improved from 62% (untreated) to 76% (APPJ-treated with the scan mode) at a current density of 80 mA cm−2, an improvement of 22%. The efficiency improvement is attributed to the oxygen-containing groups and nitrogen doping introduced by N2 APPJs on the fiber surfaces of graphite felt, both of which enhance electrochemical reactivity.