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Here, a simple solvent\u2010free supramolecular polymerization for preparing chiral polyurethanes is presented by in situ induced self\u2010assembly strategy, using cellulose nanocrystals (CNCs)\u2010based isocyanate prepolymers and macromolecular polyols as precursors, achieving precise control over polymer chain assembly with spot\u2010like arrangement. More importantly, by further incorporating a \u03c0\u2010conjugated luminescent dihydroxynaphthalene molecule, CPL\u2010active flexible polyurethane films with feather\u2010like nanostructures are constructed, which promote the ordered arrangement of CNCs\u2010based isocyanate segments due to the increased spatial resistance. The \u03c0\u2500H bond network between CNCs and urethane\u2010linked benzene rings drives the self\u2010assembly, enabling higher\u2010level chiral amplification and enhanced fluorescence. Interestingly, the prepared chiral fluorescent polyurethanes display multimodal chiroptical stimuli responsiveness under various stimuli, such as temperature, solvent polarity, pH, and polarized light, due to the sensitivity of the \u03c0\u2500H bond network. This work offers new insights into designing solvent\u2010free chiral supramolecular polymers with significant chiroptical potentials.<\/jats:p>","DOI":"10.1002\/advs.202417572","type":"journal-article","created":{"date-parts":[[2025,3,12]],"date-time":"2025-03-12T02:37:54Z","timestamp":1741747074000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Solvent\u2010Free Supramolecular Polymerization for Feather\u2010Like Nanostructured Chiral Fluorescent Polyurethanes with Multimodal Chiroptical Stimuli Responsiveness"],"prefix":"10.1002","volume":"12","author":[{"given":"Huimin","family":"Duan","sequence":"first","affiliation":[{"name":"School of Textile Science and Engineering, School of Materials Science and Engineering &amp; School of Chemistry and Chemical Engineering Zhejiang Sci\u2010Tech University  Zhejiang 310018 China"},{"name":"Zhejiang Provincial Innovation Center of Advanced Textile Technology  Zhejiang 312000 China"},{"name":"Shaoxing Keqiao Research Institute of Zhejiang Sci\u2010Tech University  Zhejiang 312000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuli","family":"Li","sequence":"additional","affiliation":[{"name":"School of Textile Science and Engineering, School of Materials Science and Engineering &amp; School of Chemistry and Chemical Engineering Zhejiang Sci\u2010Tech University  Zhejiang 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinlei","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Textile Science and Engineering, School of Materials Science and Engineering &amp; School of Chemistry and Chemical Engineering Zhejiang Sci\u2010Tech University  Zhejiang 310018 China"},{"name":"Zhejiang Provincial Innovation Center of Advanced Textile Technology  Zhejiang 312000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianping","family":"Deng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Li","sequence":"additional","affiliation":[{"name":"School of Textile Science and Engineering, School of Materials Science and Engineering &amp; School of Chemistry and Chemical Engineering Zhejiang Sci\u2010Tech University  Zhejiang 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongming","family":"Qi","sequence":"additional","affiliation":[{"name":"School of Textile Science and Engineering, School of Materials Science and Engineering &amp; School of Chemistry and Chemical Engineering Zhejiang Sci\u2010Tech University  Zhejiang 310018 China"},{"name":"Zhejiang Provincial Innovation Center of Advanced Textile Technology  Zhejiang 312000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9892-0654","authenticated-orcid":false,"given":"Biao","family":"Zhao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering, College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,2,28]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201900110"},{"key":"e_1_2_7_1_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b13291"},{"key":"e_1_2_7_1_3","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adi9944"},{"key":"e_1_2_7_1_4","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202311486"},{"key":"e_1_2_7_1_5","doi-asserted-by":"publisher","DOI":"10.1002\/rpm.20230005"},{"key":"e_1_2_7_1_6","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-38801-1"},{"key":"e_1_2_7_1_7","doi-asserted-by":"publisher","DOI":"10.1038\/s41377-024-01479-1"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c13108"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202410094"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202412283"},{"key":"e_1_2_7_3_2","author":"Ai L.","year":"2024","journal-title":"Angew. 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