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Rechargeable aqueous zinc-ion batteries (ZIBs) featured with environmental friendliness, low cost, and high safety have attracted great interest but still suffer from the lack of high-performance electrodes. Herein, a facile in situ approach is developed to simultaneously introduce multivalence, increase the interlayer water content, and expand the interlayer distance in hydrated V₂O₅. These structural modulations endow the as-obtained layer-expanded V₂O₅ 2.2H₂O (E-VO) nanosheets with faster charge transfer kinetics, more Zn²⁺ storage space, and higher structural stability than precursor V₂O₅. Besides, a unique flexible Zn/stainless steel (Zn/SS) mesh composite anode with low polarization and uniform Zn stripping/plating behavior is fabricated, which alleviates the Zn dendrite growth. As cathode for aqueous ZIBs, E-VO exhibits high reversible capacity (450 mAh g⁻¹ at 0.1 A g⁻¹), good rate capability (222 …