obstacles, such as energy instability and difficulties connecting to the high-voltage line transmission network. An effective solution is to develop low-cost and highefficiency large-scale energy storage equipment to use with such energy sources. [1][2][3][4][5] In electrochemical energy storage technologies, such as Li-ion batteries, Pb-acid batteries, and flow batteries, flow batteries, especially vanadium redox flow batteries (VRFBs), have attracted interest due to their flexible energy and power density design, low cost, lack of cross contamination, and long cycle life. Unlike other liquid-flow batteries, the phenomenon of positive and negative electrode liquid cross contamination does not occur in the recycling process of VRFBs because the positive and negative electrolytes are both based on vanadium ions. [3,[6][7][8][9][10] VRFBs mainly consist of battery stacks and positive and negative electrolyte tanks. The positive/negative electrolyte is pumped into the stack and reacts at the electrodes (Equations (1) and (2)). A Nafion-series membrane separates the cathode and anode and has a strong influence on the coulombic efficiency and energy efficiency (EE) of the battery. Therefore, an excellent vanadium battery membrane should not only ensure the passage of hydrogen ions but also limit the transmission of vanadium ions. [11][12][13][14][15] When the electronic gains and losses of VO 2+ /VO 2 + and V 2+ /V 3+ couples occur, the electrodes play an important catalytic role and provide a site for chemical reactions. Therefore, the catalytic activity of the electrode is very important for the capacity and efficiency of VRFBs VO H O VO 2H e 1.00 V vs NHE 2 2 2 E o + + + = + + + −There are two main materials that can be used as VRFB electrodes, metals and carbon-based materials. Metal electrodes are mainly precious metals, which have high catalytic activity, but their high cost and poor stability limit their commercial application. In practical applications, carbon-based materials, such as carbon cloth and graphite felt (GF), which are based on good mechanical strength and electrolyte resistance, are commercially available. However, the smooth and uniform surfaces of carbon-based materials lack sufficient catalytic sites, resulting in poor catalytic activity and limiting the further improvement of battery performance. [2,[16][17][18] Many researchers have tried Surface-wrinkle-modified graphite felt (GF) with abundant N and O is prefabricated by a hydrothermal method followed by calcination, and its surface morphology, elemental composition, and electrochemical properties are characterized by scanning electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, cyclic voltammetry, electrochemical impedance spectroscopy, and charge/discharge tests. The highly folded coating has excellent wettability, abundant catalytic sites, a fast ion-diffusion rate, ultralow interface transfer resistance, and high catalytic activity for VO 2+ /VO 2 + and V 2+ /V 3+ reaction couples. Compared with the original GF, t...