AbstractEmerging as a leading contender for economical, high‐security grid‐scale energy storage, rechargeable aqueous zinc‐ion batteries (AZIBs) are currently facing the challenge in its progression due to the absence of cathode materials with high energy density. In this study, we design a V2O5 ⋅ nH2O, GO and CNTs composite (HVO/GO‐CNTs) film through freeze‐drying and vacuum filtration. This binder‐free cathode for AZIBs exhibits remarkable electrochemical performance, featuring a high capacity of 387 mAh g−1 at 0.2 A g−1 and a high capacity retention of 82.6 % after 1000 cycles at 1 A g−1. This investigation offers a promising approach to electrode material design for the advancement of high‐performance AZIBs.