Rechargeable aqueous zinc-ion batteries (ZIBs) have recently received increasing attention due to their high safety, low cost, and material abundance. Nevertheless, finding a suitable cathode material with a high capacity and good stability remains a challenge. To solve this problem, we prepared vanadium pentoxide microspheres with high performance through a one-step spray-drying process. As confirmed by SEM and laser granulometry, microspheres in the range of 1–10 µm are obtained and result from the agglomeration of commercial nanoparticles. A comparative study with commercial V₂O₅ is realized and shows the benefit of the architecture design of vanadium pentoxide on the electrochemical performance of ZIBs. Spray-dried V₂O₅ delivers remarkably high capacities of 495 mAh g⁻¹ and 240 mAh g⁻¹ at low (0.1 A g⁻¹) and high current density (5 A g⁻¹) respectively, excellent rate capability, and good stability. Excellent capacity retention of 93 % is observed after 1000 cycles at high current density. The experimental results suggest a promising potential for V₂O₅ microspheres as cathode material in aqueous zinc-ion batteries.