Aqueous zinc-ion batteries (ZIBs) represent a promising frontier for energy storage system, yet the viability is limited by the scarcity of robust cathodes capable of accommodating divalent Zn²⁺ ions. Herein, we developed a deliberate structural-modulation strategy to yield a unique Zn_0.62Li_1.2V₂(PO₄)₃ (ZLVP)cathode by controllable chemical pre-zincification. The ZLVP delivers a reversible capacity of 101.5 mAh·g⁻¹ via a two-phase reaction, and exhibits a high voltage of 1.51 V owing to the strong inductive effect of the PO₄³⁻ framework. Remarkably, the minimal volume variation of only 4.3% during cycling underpins outstanding structural stability, leading to negligible capacity degradation over 5000 cycles. Furthermore, two rocking-chair-type full cells employing either an organic anode (9,10-AQ) or an inorganic anode (TiS₂) were assembled, demonstrating the feasibility of the ZLVP cathode. These findings establish a reliable foundation for advancing the practical implementation of aqueous ZIBs.