Ordered Organic–Inorganic Dual‐Layer Synergistic Interfaces on Zinc Anodes Enable High‐Performance Zinc Metal Batteries

ABSTRACT A stable zinc (Zn) metal anode (ZMA) is critical for the practical application of aqueous zinc metal batteries (AZMBs), yet challenges such as dendrite formation and side reactions severely hinder long‐term cycling. In this study, we report a well‐ordered organic–inorganic dual‐layer synergistic interface (OIDL) to construct a high‐efficiency ZMA (denoted as OIDL@Zn). OIDL interface is composed of a bottom ZnF 2 ‐rich inorganic layer and a top organic Zn‐ligand complex layer in situ grown on the Zn surface. The organic layer with polar functional groups renders homogeneous and enhanced Zn 2+ flux, compressed electric double layer (EDL) structure, and facilitated Zn 2+ desolvation, thereby enabling uniform Zn deposition and suppressing parasitic reactions. ZnF 2 layer with excellent mechanical stability simultaneously provides efficient Zn 2+ transport pathways and suppresses dendrite growth. Consequently, OIDL@Zn anodes exhibit remarkable cycling stability (over 3000 h at 1 mA cm −2 , over 4500 cycles at 20 mA cm −2 ). A high average Coulombic efficiency (CE) of 99.38% is achieved by OIDL@Zn||Cu cells during 2000 cycles for Zn plating/stripping. Assembled OIDL@Zn||MnO 2 full cells deliver an initial discharge capacity of 231.6 mA h g −1 with a highly improved capacity retention of 86.8% after 2500 cycles at 1 C, and pouch cell tests further validate its stability and practical applicability.