Neutral aqueous rechargeable zinc-ion batteries are receiving continuous attention because of their advantages of low cost, high safety, environmental friendliness, and high performance, which are difficult to attain with current organic electrolyte-based batteries. In this work, a high-performance aqueous Zn-ion battery based on the organic pigment 3,4,9,10-perylene-tetracarboxylic acid dianhydride (PTCDA) is developed. An electrochemical test shows that the PTCDA possesses a high specific discharge capacity of 136 mAh·g⁻¹ at a current density of 10 mA·g⁻¹. Moreover, the PTCDA cathode displays a good rate performance (77 mAh·g⁻¹ at 1 A·g⁻¹) and an excellent cycle life with a capacity retention of 80% after 2000 cycles. Furthermore, electrochemical analysis and structural characterization originally reveal that the PTCDA cathode undergoes a sequential Zn²⁺ and H₃O⁺ insertion and extraction process, which is reversible and cycling stable. Graphical abstract: [Figure not available: see fulltext.]