In an all-vanadium redox flow battery (VRFB), redox reaction occurs on the fiber surface of the graphite felts. Therefore, the VRFB performance highly depends on the characteristics of the graphite felts. Although atmospheric pressure plasma jets (APPJs) have been applied for surface modification of graphite felt electrode in VRFBs for the enhancement of electrochemical reactivity, the influence of APPJ plasma reactivity and working temperature (by changing the flow rate) on the VRFB performance is still unknown. In this work, the performance of the graphite felts with different APPJ plasma reactivity and working temperatures, changed by varying the flow rates (the conditions are denoted as APPJ temperatures hereafter), was analyzed and compared with those treated with sulfuric acid. X-ray photoelectron spectroscopy (XPS) indicated that the APPJ treatment led to an increase in O-/N-containing functional groups on the GF surface to ~21.0% as compared to ~15.0% for untreated GF and 18.0% for H 2SO 4-treated GF. Scanning electron microscopy (SEM) indicated that the surface morphology of graphite felt electrodes was still smooth, and no visible changes were detected after oxidation in the sulfuric acid or after APPJ treatment. The polarization measurements indicated that the APPJ treatment increased the limiting current densities from 0.56 A·cm −2 for the GFs treated by H 2SO 4 to 0.64, 0.68, and 0.64 A·cm −2, respectively, for the GFs APPJ-treated at 450, 550, and 650 °C, as well as reduced the activation overpotential when compared with the H 2SO 4-treated electrode. The electrochemical charge/discharge measurements showed that the APPJ treatment temperature of 550 °C gave the highest energy efficiency of 83.5% as compared to 72.0% with the H 2SO 4 treatment.