Abstract: | Rechargeable aqueous zinc‐ion batteries hold great promise for potential applications in large‐scale energy storage, but the reversible insertion of bivalent Zn2+ and fast reaction kinetics remain elusive goals. Hence, a highly reversible Zn/VNx Oy battery is developed, which combines the insertion/extraction reaction and pseudo‐capacitance‐liked surface redox reaction mechanism. The energy storage is induced by a simultaneous reversible cationic (V3+ ? V2+) and anionic (N3? ? N2?) redox reaction, which are mainly responsible for the high reversibility and no structural degradation of VNxOy. As expected, a superior rate capability of 200 mA h g?1 at 30 A g?1 and high cycling stability up to 2000 cycles are achieved. This finding opens new opportunities for the design of high‐performance cathodes with fast Zn2+ reaction kinetics for advanced aqueous zinc‐ion batteries. |