Due to the energy crisis and environmental pollution, aqueous Zn-based batteries stand out. However, aqueous Zn-based batteries still suffer from anode and cathode issues, leading to low rate capability and poor long-term cycling performance. Herein, a novel organic compound 2,3-diethylbenzo[g]quinoxaline-5,10-dione (DEBQ) is synthesized and used as the cathode active material for aqueous Zn-organic batteries. Li2SO4, Na2SO4, and MgSO4 were added to the commonly used ZnSO4 aqueous electrolyte to simultaneously regulate the anode and cathode interfaces. For the Zn anode side, side reactions such as HER and corrosion are inhibited, and Zn nucleation and uniform deposition are promoted. For the DEBQ cathode side, H+, Zn2+, and additive cations (Na+, Li+, and Mg2+) cocoordinate with the active sites (C=O and C=N) of DEBQ. Among them, the introduction of Na+ in the electrolyte can improve the specific capacity of batteries and reaction kinetics and provide a more stable cycle life over 120,000 cycles. This work provides a simple way to improve the performance of aqueous Zn-organic batteries by simultaneously regulating the interfaces of both electrodes.