A Geomag-inspired dynamically reconfigurable POSS framework is constructed to form an antifatigue solid electrolyte interphase (SEI) for lithium metal anodes. The rigid POSS nanocages and reversible hydrogen-bonded junctions enable adaptive stress dissipation and stable Li + transport during repeated plating/stripping, thereby suppressing dendrite growth, mitigating interfacial fatigue accumulation, and significantly enhancing long-term electrochemical stability. ABSTRACT Lithium metal anodes are fundamentally limited by mechanical fatigue and structural instability of the solid electrolyte interphase (SEI) during repeated plating and stripping. Here, we introduce a stress-adaptive molecular interphase featuring autonomously reconfigurable ion-transport channels inspired by modular “Geomag”-like architecture. The interphase is constructed from polyhedral oligomeric silsesquioxane (POSS) nanocages bridged by reversible melamine-mediated hydrogen bonds, forming dynamic secondary junctions that enable stress-triggered disconnect–reconnect behavior. This reversible connectivity allows the SEI to dissipate local strain while actively opening and closing Li + transport pathways, thereby homogenizing ion flux and stabilizing the interfacial electric field. Antifatigue architecture effectively suppresses dendrite nucleation and prolongs interfacial stability. Symmetric Li || Li and Li || Cu cells verify enhanced reversibility, while Li || LTO full cells sustain ultralong cycling exceeding 2000 h. Pouch-type lithium metal cells further demonstrate stable electrochemical performance under practical conditions. This work establishes a general molecular design paradigm for autonomously self-regulating SEIs toward durable lithium metal cells.

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