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Herein, we present a molecular\u2010level design of a dynamically interlocked dual\u2010stiffness interphase to break this limit, utilizing an aramid nanofiber\/silica double\u2010network architecture. Unlike traditional physical blending, this interphase is governed by a bidirectional hydrogen\u2010bonding network. Through deep spectroscopic investigations, we reveal that this strong interfacial interaction triggers an intramolecular proton transfer and electronic redistribution within the ANFs. More intriguingly, this supramolecular interaction drives a rare and critical structural phase transition within the inorganic network, transforming flexible six\u2010membered siloxane rings (SiO)\n                    <jats:sub>6<\/jats:sub>\n                    into rigid four\u2010membered rings (SiO)\n                    <jats:sub>4<\/jats:sub>\n                    . Macroscopically, this chemical interphase is integrated into a biomimetic skin\u2010core aerogel fiber. The bimodal chemical interactions\u2014static anchoring and dynamic silanol\u2010mediated slippage\u2014synergistically endow the hybrid with an ultrahigh modulus (1.15\u00a0GPa) and exceptional toughness (8.1\u00a0MJ m\n                    <jats:sup>\u22123<\/jats:sup>\n                    ), while preserving intrinsic extreme\u2010temperature stability. This chemically driven dynamic phase\u2010reconfiguration mechanism establishes a universal theoretical framework for interphase engineering, offering profound insights for the precise construction of high\u2010performance multifunctional nanocomposites.\n                  <\/jats:p>","DOI":"10.1002\/anie.7495552","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T10:39:24Z","timestamp":1788259164000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Supramolecular Engineering of Dynamically Interlocked Dual\u2010Stiffness Interphase for Biomimetic Strong and Tough Double Network Aerogel"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5620-784X","authenticated-orcid":false,"given":"Zi\u2010Meng","family":"Han","sequence":"first","affiliation":[{"name":"Division of Nanomaterials &amp; Chemistry Department of Chemistry New Cornerstone Science 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