Tianyi Wang, Jiahui Lu, Wei Gu, Jianfei Shi, Yuting Qin, Jian Yang, Di He, Zixia Lin, Jiabao Li, Bing Sun, Guoxiu Wang, Chengyin Wang
Aqueous zinc (Zn) metal cells are promising candidates for large-scale energy storage owing to their intrinsic safety and low cost. However, their practical application remains limited by uncontrolled Zn dendrite growth and hydrogen-evolution-induced corrosion. Here, we present a collagen-engineered strategy that harnesses the natural triple-helix architecture of collagen to construct collagen-coated cotton fiber (COL@COT) separators capable of continuous collagen release and dynamic interfacial regulation. The ordered triple-helix chains enable directional Zn2+ migration through interconnected ion channels bridging the anode, electrolyte, and cathode, while the released collagen molecules migrate under the electric field to assemble a self-adaptive organic-inorganic SEI. During prolonged cycling, inner layer collagen undergoes a secondary-structure evolution from the triple-helix to β-sheet domains, giving rise to a multilayered SEI with both flexibility and rigidity that maintains long-term interfacial stability. This adaptive interphase lowers Zn-ion desolvation barriers, directs (002)-oriented Zn deposition, and suppresses water-induced side reactions, thereby ensuring dendrite-free and durable Zn plating/stripping. As a result, Zn||Zn symmetric cells exhibit ultralong cycling stability over 2200 h at 5 mA cm-2 and 1 mAh cm-2. This work introduces a secondary-structure-programmed biomolecular approach for interphase engineering, bridging structural biology and electrochemistry to inspire the design of sustainable, bio-derived energy storage systems.