Chiral Coordination Interphase‐Mediated Ion Regulation and Shuttle Suppression for Stable Zinc–Iodine Batteries

ABSTRACT The practical deployment of aqueous zinc–iodine (Zn–I 2 ) batteries is severely hampered by coupled challenges of Zn anode irreversibility and polyiodide shuttle effect, leading to rapid capacity decay and shortened cycle life. Inspired by the ordered ion‐transport characteristics of low‐dimensional chiral metal–organic coordination polymers, we report a zinc nicotinate (NAZ) chiral coordination interphase that forms spontaneously in‐situ on Zn anode, with integrated functionalities of Zn 2+ ion regulation, interfacial corrosion suppression, and polyiodide trapping. Real‐time spectroscopic tracking and theoretical calculations reveal that NAZ interphase exerts synergistic effects: its chiral coordination framework provides strong zincophilicity to homogenize Zn 2+ flux and promote uniform nucleation; meanwhile, the hydrophilic nature of its backbone reduces water accessibility to minimize side reactions, while its capacity to selectively adsorb polyiodides effectively alleviates the shuttle effect. Benefiting from these merits, the NAZ@Zn symmetric cells deliver exceptional cycling stability over 3500 h at 1 mA cm −2 and 1800 h at 5 mA cm −2 . When paired with an I 2 cathode, the full cell retains a reversible capacity of 169.8 mAh g −1 after 18000 cycles. This work highlights the untapped potential of chiral coordination polymers for interphase engineering and establishes a general strategy for stabilizing metal anodes in aqueous energy‐storage systems.