To increase the electrocatalytic activity of graphite felt (GF) electrodes in vanadium redox flow batteries (VRFBs) toward the VO2+/VO2+ redox couple, we prepared a stable, high catalytic activity and uniformly distributed hexagonal Ta2O5 nanoparticles on the surface of GF by varying the Ta2O5 content. Scanning electron microscopy (SEM) revealed the amount and distribution uniformity of the electrocatalyst on the surface of GF. It was found that the optimum amount and uniformly immobilized Ta2O5 nanoparticles on the GF surface provided the active sites, enhanced hydrophilicity, and electrolyte accessibility, thus remarkably improved electrochemical performance of GF. In particular, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) results showed that the Ta2O5-GF nanocomposite electrode with a weight percentage of 0.75 wt % of Ta2O5 to GF exhibited the best electrochemical activity and reversibility toward the VO2+/VO2+ redox reaction, when compared with the other electrodes. The co...