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Here, we demonstrate a path toward resolving these dilemmas by engineering a novel porous liquid\u2010based electrolyte that decouples the essential catalytic activity from deleterious side reactions via microenvironment modulation. The macrocyclic molecular host leverages its intrinsic structural duality\u2014dynamically coordinating a subpopulation of Zn\n                    <jats:sup>2+<\/jats:sup>\n                    ions to reconstruct their local solvation environment, while utilizing its bulky scaffold to impose steric constraints on polyiodide association and accessibility. This architectural strategy promotes the participation of transient soluble sulfur intermediates and facilitates a more reversible interfacial S\u2194ZnS conversion, delivering a higher discharge plateau of 0.77\u00a0V versus Zn\n                    <jats:sup>2+<\/jats:sup>\n                    \/Zn and a reduced cell polarization of 0.38\u00a0V at 0.2 A g\n                    <jats:sup>\u20121<\/jats:sup>\n                    . Simultaneously, it mitigates mediator\u2010induced zinc corrosion, enabling an 89% capacity retention over 1000 cycles at 1 A g\n                    <jats:sup>\u20121<\/jats:sup>\n                    . These findings, based on both experimental and theoretical evidence, elucidate the critical role of steric regulation in electrolyte design, establishing a clear direction for realizing a paradigm shift in aqueous metal\u2010chalcogen batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.7425389","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T04:06:57Z","timestamp":1791518817000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Crown Ether\u2010Engineered Porous Liquid\u2010Based Electrolytes Decouple Redox Kinetics and Stability in Zinc\u2013Sulfur Batteries"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4394-0919","authenticated-orcid":false,"given":"Xin","family":"Liu","sequence":"first","affiliation":[{"name":"Songshan Lake Materials Laboratory (SLAB)  Dongguan China"},{"name":"Department of Energy and Process Engineering Faculty of 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