Hierarchically Structured Artificial SEI with Interlayer Electronic Coupling for High‐Performance Aqueous Zinc Batteries

ABSTRACT Aqueous zinc‐ion batteries (AZIBs) are considered promising candidates for large‐scale energy storage owing to their intrinsic safety and low cost. However, challenges such as dendrite growth, parasitic reactions, and unstable interfaces severely limit their performance. Herein, we reported a multifunctional artificial SEI layer with an engineered armored petalosphere heterostructure (ZnO@MX‐DE), constructed via a multi‐step strategy involving ZIF‐8 templating, MXene coating, ZnO converting, and dickite nanosheet compositing. This heterostructure induced significant interfacial electron reconstruction, wherein electrons migrated from Zn/Ti centers to oxygen‐rich dickite nanosheet, effectively adsorbing Zn ²⁺ and repelling SO ₄ ²⁻ . The resultant SEI layer exhibited ultrahigh ionic conductivity (20.26 mS cm ⁻¹ ) and Zn ²⁺ transference number (0.89), enabling Zn//Zn cells to stably cycle over 4000 h. Remarkably, the Zn//MnO ₂ full cell delivered 77.10% capacity retention after 700 cycles at 300 mA g ⁻¹ and achieved 40 000 cycles at 30 A g ⁻¹ . This work offers a rational interfacial engineering strategy integrating morphological design and electronic tuning, promoting the development of high‐performance AZIBs.