<p>Owing to their inherent advantages of safety, eco-friendliness, and low cost, aqueous zinc-ion batteries (AZIBs) are regarded as promising candidates for next-generation large-scale energy storage systems. However, the practical application of V₂O₅, a typical layered vanadium-based cathode, in high-performance AZIBs suffers from its low intrinsic electronic conductivity, sluggish Zn²⁺ diffusion kinetics, and structural collapse during cycling. Herein, we prepared an NH₄–P–V₂O₅ cathode via a facile hydrothermal strategy, in which the V₂O₅ matrix was modified using ammonium dihydrogen phosphate (NH₄H₂PO₄). This modification retains the layered framework of V₂O₅ and is associated with a slight expansion of the interlayer spacing, which is favorable for Zn²⁺ diffusion. As a result, the NH₄–P–V₂O₅ electrode shows improved electrochemical performance. It delivers a high reversible capacity of 465.4 mAh g⁻¹ at 100&#xa0;mA&#xa0;g⁻¹ and maintains a capacity of 50.47 mAh g⁻¹ after 1500 cycles even at a high current density of 1000&#xa0;mA&#xa0;g⁻¹, which is higher than that of pristine V₂O₅ under the same conditions. This work provides a simple strategy for improving the electrochemical performance of V₂O₅-based materials and offers useful insights for the design of cathodes for AZIBs.</p>