Structure‐Kinetic Coordination for Reconstructing Anode‐Molecular Interfaces Toward Stable and Efficient Aqueous Zinc‐Ion Batteries

ABSTRACT Uncontrolled interfacial reactions and sluggish ion‐transfer kinetics at zinc metal anodes remain fundamental obstacles for aqueous zinc‐ion batteries. Conventional organic interfacial modifiers can suppress parasitic reactions but inevitably impose kinetic penalties, leading to a long‐standing trade‐off between interfacial stability and fast Zn 2+ transport. Here we propose a previously unexplored concept, termed structure‐kinetic coordination (SKC), which simultaneously reconstructs the anode‐molecular interface and accelerates interfacial charge‐transfer kinetics through the cooperative action of halide ions and organic molecules. Using iodide ions as a prototypical kinetic coordinator, we demonstrate that halide pre‐adsorption electrostatically templates the ordered assembly of soybean peptide molecules into a dense and defect‐free adsorption layer, while concurrently reshaping the Zn 2+ solvation structure to promote rapid water desolvation. This coordinated regulation bridges the intrinsic conflict between interfacial protection and ion transport, leading to uniform Zn nucleation, suppressed dendrite growth, and mitigated parasitic reactions. The resulting interface enables highly reversible Zn plating/stripping with markedly reduced energy barriers and exceptional long‐term stability under demanding conditions. Importantly, the SKC strategy is not limited to a specific molecular additive or halide species, but represents a broadly applicable interfacial design principle that can be extended to diverse organic molecule‐halide combinations in aqueous metal batteries.