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Here we propose a strategy\u2014\u201cfrustrated non\u2010covalent complexation\u201d\u2014inspired by frustrated Lewis pairs to overcome this limitation. This is achieved by installing sterically hindering isopropyl groups adjacent to directional squaramide hydrogen\u2010bonding motifs. Relative to a nonfrustrated control, this design not only generates more loosely packed hydrogen\u2010bonded domains but also shifts the dominant interactions from squaramide\u2013squaramide to squaramide\u2013ester hydrogen bonding. The frustrated system yields a 4.3\u2010fold increase in mechanical toughness in the resulting supramolecular glass, facilitated by efficient energy dissipation through reversible hydrogen\u2010bond rupture. It also enhances interfacial adhesion, functioning as an effective impact\u2010resistant coating that mitigates substrate fracture. Overall, this work establishes frustrated noncovalent complexation as a powerful paradigm for designing high\u2010performance supramolecular glass materials.<\/jats:p>","DOI":"10.1002\/anie.202519907","type":"journal-article","created":{"date-parts":[[2025,10,11]],"date-time":"2025-10-11T11:26:29Z","timestamp":1760181989000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Tough Supramolecular Glasses Enabled by Frustrated Non\u2010Covalent Complexation"],"prefix":"10.1002","volume":"64","author":[{"given":"Jianfei","family":"Ma","sequence":"first","affiliation":[{"name":"Department of Vascular Surgery The First Affiliated Hospital of USTC and Key Laboratory of Precision and Intelligent Chemistry University of Science and Technology of China  Hefei Anhui 230026 P.R. 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