This study investigates the use of charged organic carboxylic acid ligands to enhance the performance of vanadium oxide (VO) electrodes in aqueous zinc-ion batteries (AZIBs). The negatively charged carboxylic acid groups in these ligands neutralize Zn2+, reduce electrostatic repulsion, and improve electrochemical kinetics. The intercalated organic molecules increase the interlayer spacing of VO, which is crucial for enhancing the material's properties. Among the tested ligands, 0.028EDTA·0.28NH4+·V2O5·0.069H2O showed the best performance as a cathode, with a high specific capacity (464.6 mAh g−1 at 0.5 A g−1) and excellent rate capability (324.4 mAh g−1 at 10 A g−1). Even at a current density of 20 A g−1, the specific capacity after 2000 charge/discharge cycles was 215.2 mAh g−1, with a capacity retention of 78%. The study demonstrates that modulating the electrostatic repulsion and interlayer spacing through the intercalation of organic ligands can significantly enhance the properties of vanadium-based materials, making them suitable for AZIBs.This study investigates the use of charged organic carboxylic acid ligands to enhance the performance of vanadium oxide (VO) electrodes in aqueous zinc-ion batteries (AZIBs). The negatively charged carboxylic acid groups in these ligands neutralize Zn2+, reduce electrostatic repulsion, and improve electrochemical kinetics. The intercalated organic molecules increase the interlayer spacing of VO, which is crucial for enhancing the material's properties. Among the tested ligands, 0.028EDTA·0.28NH4+·V2O5·0.069H2O showed the best performance as a cathode, with a high specific capacity (464.6 mAh g−1 at 0.5 A g−1) and excellent rate capability (324.4 mAh g−1 at 10 A g−1). Even at a current density of 20 A g−1, the specific capacity after 2000 charge/discharge cycles was 215.2 mAh g−1, with a capacity retention of 78%. The study demonstrates that modulating the electrostatic repulsion and interlayer spacing through the intercalation of organic ligands can significantly enhance the properties of vanadium-based materials, making them suitable for AZIBs.