Yonghang Wei, Zheng Wang, Jun Li, Sheng Mao, Fuyi Li, Xinyi Zhou, Xiaoxuan Guo, Yun Lu
ABSTRACT Aqueous zinc‐ion batteries (AZIBs) operate stably at low depth of discharge (DOD) but suffer severe Zn 2+ transport imbalance, hydrogen evolution, and plating/stripping at high DOD (> 70%). Here, we present a radial wood‐based hierarchical heterogeneous interconnected structure (HHIS) electrolyte. HHIS is without low‐tortuosity channels, but during cycling, Zn 2+ predominantly migrates along laterally oriented vessels, fibers, and rays via pit coordination, ensuring uniform deposition. Leveraging these synergistic effects, HHIS stabilizes the Zn anode under high current, enabling > 9000 h of cycling and > 3300 h at 83.1% DOD, surpassing previous reports. This work directly converts wood into a high‐performance electrolyte and establishes a HHIS design strategy for addressing high‐DOD instability in AZIBs and advancing electrolyte commercialization.