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Side reactions on zinc metal (Zn) anodes are formidable issues that cause limited battery life of aqueous zinc‐ion batteries (AZIBs). Here, a facile and controllable layer‐by‐layer (LbL) self‐assembly technique is deployed to construct an ion‐conductive and mechanically robust electrolyte/anode interface for stabilizing the Zn anode. The LbL film consists of two natural and biodegradable bio‐macromolecules,...