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Herein, this bottleneck is overcome by adopting a quartet\u2010wise approach of constructing H\u2010bonds instead of the traditional pairwise method. Thus, large multiple hydrogen bonds can be easily established, and the supramolecular interactions are further reinforced. Especially, when such multiple H\u2010bond motifs are embedded in polymers, four macromolecular chains\u2014rather than two as usual\u2014are tied, distributing the applied stress over a larger volume and more significantly improving the overall mechanical properties. Proof\u2010of\u2010concept studies indicate that the proposed intermolecular multiple H\u2010bonds (up to duodecuple) are readily introduced in polyurethane. A record\u2010high tensile strength (105.2\u00a0MPa) is achieved alongside outstanding toughness (352.1 MJ m\n                    <jats:sup>\u22123<\/jats:sup>\n                    ), fracture energy (480.7 kJ m\n                    <jats:sup>\u22122<\/jats:sup>\n                    ), and fatigue threshold (2978.4 J m\n                    <jats:sup>\u22122<\/jats:sup>\n                    ). Meantime, the polyurethane has acquired excellent self\u2010healability and recyclability. This strategy is also applicable to nonpolar polymers, such as polydimethylsiloxane, whose strength (15.3\u00a0MPa) and toughness (50.3 MJ m\n                    <jats:sup>\u22123<\/jats:sup>\n                    ) are among the highest reported to date for silicones. This new technique has good expandability and can be used to develop even more and stronger polymers.\n                  <\/jats:p>","DOI":"10.1002\/adma.202406574","type":"journal-article","created":{"date-parts":[[2024,6,21]],"date-time":"2024-06-21T10:34:05Z","timestamp":1718966045000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":102,"title":["Imparting Ultrahigh Strength to Polymers via a New Concept Strategy of Construction of up to Duodecuple Hydrogen Bonding among Macromolecular Chains"],"prefix":"10.1002","volume":"36","author":[{"given":"Yi Wei","family":"Wen","sequence":"first","affiliation":[{"name":"Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education GD HPPC Lab School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Li","sequence":"additional","affiliation":[{"name":"Key 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Ministry of Education GD HPPC Lab School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center  Jieyang 515200 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