Synergistic Organic–Inorganic Interface Engineering for Stable Zinc Metal Anodes in Aqueous Batteries

ABSTRACT In aqueous zinc‑ion batteries (AZIBs), uncontrolled dendrite growth and parasitic corrosion reactions critically limit long‑term stability. Constructing a robust organic–inorganic solid electrolyte interphase (SEI) has emerged as an effective strategy; however, the mechanistic origin of Zn‐anode stabilization remains insufficiently understood. Here, we in situ construct an ultrathin organic–inorganic hybrid SEI (Zn‐S‐RCOOH) on Zn using a multifunctional organic acid, mercaptosuccinic acid (MSA). The COOH‑rich organic outer layer restructures the interfacial hydrogen‑bond (HB) network, lowers H 2 O activity, and accelerates desolvation, whereas the inner ZnS layer provides fast Zn 2+ migration pathways, collectively enhancing reaction kinetics and promoting (002) oriented Zn deposition. Owing to these synergistic effects, dendrite formation and corrosion are effectively inhibited. The MSA/Zn electrode operates stably for over 2400 h at 10 mA cm −2 and 5 mAh cm −2 , and maintains>500 h stability even at a high depth of discharge (DOD, 81 %). Moreover, MSA/Zn||MnO 2 full cells exhibited capacities of ∼189.7 and 142 mAh g −1 with high‐capacity retention (99.18 % and 97.55 %) at 0.3 and 1 A g −1 , respectively. So, our findings proposed a rational interfacial‐engineering strategy for designing durable Zn metal anodes and advancing high‐performance aqueous zinc‐ion batteries.