AbstractRedox‐active organic materials, as a new generation of sustainable resources, are receiving increasing attention in zinc‐ion batteries (ZIBs) due to their resource abundance and tunable structure. However, organic molecules with high potential are rare, and the voltage of most reported organic cathode‐based ZIBs is less than 1.2 V. Herein, we explored the redox process of p‐type organics and figured out the relationship between energy change and voltage output during the process. Then, we proposed a dual‐step strategy to effectively tune the energy change and eventually improve the output voltage of the organic electrode. Combining the regulation of the electron cloud of organic molecules and the manipulation of the solvation structure, the output voltage of an organosulfur compound based ZIB was greatly increased from 0.8 V to 1.7 V. Our results put forward a specific pathway to improve the working voltage and lay the foundation for the practical application of organic electrodes.