Adhesive Tape‐Inspired Polymer Coatings Enable Record‐Stable Zinc Anodes for High‐Rate Aqueous Batteries

The development of stable zinc anodes is critical for advancing high-rate, long-life aqueous zinc batteries. Here a tape-inspired anode modification is reported using a poly (methyl methacrylate)-grafted natural rubber (NRAc) copolymer as a conformal protective coating. The microphase-separated architecture integrates elastic, hydrophobic NR domains with Zn²⁺-coordinating PMMA nanodomains, forming mechanically adaptive and ion-selective channels. Density functional theory and microscopy reveal that Zn²⁺ preferentially binds to PMMA, lowering desolvation barriers and biasing deposition toward the stable (002) facet. This dual mechanical-chemical regulation suppresses dendrite growth and parasitic hydrogen evolution, while maintaining intimate interfacial contact under dynamic cycling. As a result, NRAc@Zn symmetric cells achieve unprecedented cycling lifetimes exceeding 32,000 cycles, while Zn||V₂O₅ full cells deliver stable operation at current densities up to 10 A g^-1. Scaling to a 1.5 Ah pouch cell demonstrates the practical feasibility of the approach. This work establishes polymer microphase engineering, inspired by the multifunctionality of adhesive tapes, as a versatile strategy to stabilize Zn anodes and advance the deployment of aqueous Zn batteries for large-scale energy storage.