Bioinspired Halloysite Nanotubes as a Triple‐Synergistic Buffer Layer for Highly Stable Zinc Metal Anodes

Aqueous zinc metal batteries suffer from sluggish desolvation kinetics and non‐uniform ion flux, which synergistically induce rampant dendrite formation and detrimental side reactions. Inspired by the dynamic ion‐regulation of plant roots, a bioinspired halloysite nanotube (HNT) buffer layer is designed to construct a stable, fast‐ion‐transport interphase, resolving the stability‐conductivity trade‐off of traditional coatings. Experimental and theoretical analyses reveal that the HNT layer regulates interfacial Zn 2+ via a triple‐synergistic mechanism. The polar Si─O groups enrich Zn 2+ to form a localized ion reservoir that eliminates concentration polarization, while strong electrostatic interactions expel coordinated water to promote desolvation and suppress hydrogen evolution. Additionally, the unique tubular architecture and charge redistribution homogenize the Zn 2+ flux for dense, dendrite‐free deposition. Consequently, the HNTs@Zn anode delivers exceptional stability over 2000 h at 0.25 mA cm −2 /0.125 mAh cm −2 and 800 h at 10 mA cm −2 /5 mAh cm −2 . Furthermore, Zn||AC (AC: activated carbon) full cells achieve over 10,000 stable cycles with markedly enhanced rate capability. This bioinspired, mineral‐based strategy provides a scalable and highly effective paradigm for long‐lifespan aqueous metal batteries.