A Chemical Sewing Enabled All‐In‐One Control Interface for Robust Zinc Metal Anodes

Abstract Developing artificial protective layers is an effective strategy to address the issue of dendrites for aqueous Zn‐metal batteries (ZMBS). However, drawbacks such as rough microscopic morphology, excessive thickness, and single functionality remain, limiting the attainment of a stable zinc anode. Herein, a novel multifunctional organic–inorganic hybrid artificial protective layer is produced by splicing inorganic fragments onto organic materials in situ using a chemical sewing. The protective layer is well‐compatible and also retains the function of organic and inorganic materials, which not only inhibits dendrite production but also alleviates Zn corrosion. The Si─OH bond of the zincophilic group enables planar Zn deposition while forming hydrogen bonds with water, suppressing water activity near the anode and reducing the hydrogen evolution reaction. As expected, the Zn||Zn symmetric cell with a protective layer provides high cycling stability of more than 1960 h at 1 mA cm⁻², which is about 28 times higher than that of the symmetric cell assembled without the protective layer. More importantly, a Zn||V₂O₅ full cell with an ultra‐long lifetime has been achieved with an artificial protective layer. This work provides a potential viable path to achieve long‐lived ZMBS.