Mechanically Adaptive Ultrathin Interphase Inspired by Sliding Filament for Highly Reversible Zinc Metal Anodes

Dendrite growth and interfacial instability fundamentally limit the reversibility of aqueous zinc metal batteries. Artificial solid electrolyte interphases (SEIs) are typically constrained by an intrinsic trade‐off between mechanical rigidity for dendrite suppression and flexibility to accommodate volume fluctuations. Here, inspired by the sliding filament mechanism of biological muscle, we construct a mechanically adaptive ultrathin interphase that reconciles rigidity with deformability through dynamic hydrogen‐bond‐mediated stress dissipation. A nanoscale reinforced architecture, composed of rigid graphene oxide (GO) backbones interconnected by Triton‐induced sacrificial hydrogen bonds, enables controlled interlayer sliding while preserving structural integrity. The resulting ∼80 nm interphase simultaneously delivers a high Young's modulus (22.4 GPa) and tensile strain (∼12%), effectively overcoming the modulus–flexibility constraint. Meanwhile, the interphase promotes Zn 2+ desolvation and stabilizes the interfacial microenvironment. Consequently, Zn||Cu cells deliver over 10000 cycles at 5 mA cm −2 with an average coulombic efficiency (CE) of 99.93% and a cumulative capacity exceeding 10 Ah cm −2 . Zn||MnO 2 cells operated at a low N/P ratio of 2.5 exhibit markedly improved cycling stability. This work establishes a mechanically adaptive interphase design principle for stabilizing zinc metal anodes.