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Hydrogen\u2010bonded organic frameworks (HOFs) exhibit unique flexibility derived from their weak, reversible hydrogen\u2010bonding interactions; however, realizing controlled and functional flexible behavior in HOFs remains a synthetic challenge. Herein, we report a flexible hydrogen\u2010bonded organic framework,\n                    <jats:bold>HOF\u2010FJU\u2010119<\/jats:bold>\n                    , constructed from an anthracene\u2010core, that exhibits multimode guest\u2010responsive behavior. Upon activation,\n                    <jats:bold>HOF\u2010FJU\u2010119a<\/jats:bold>\n                    undergoes distinct gate\u2010opening transformations in response to CO\n                    <jats:sub>2<\/jats:sub>\n                    at 196\u00a0K and benzene vapor at room temperature. Single\u2010crystal X\u2010ray diffraction (SCXRD) and vapor adsorption isotherms reveal the emergence of new adsorption sites in the benzene\u2010loaded phase, driven by strong interactions and the flexibility of C\u2261N\u22efH\u2500C hydrogen bonds, enabling selective benzene\/cyclohexane separation. Notably, the adsorption of benzene induces a visible color change in fluorescence emission and a red shift of approximately 60\u00a0nm. Structural and density functional theory (DFT) analyses confirm increased molecular planarity, extended conjugation, and a narrowed bandgap. This work demonstrates a rare integration of selective adsorption, molecular recognition, and signal transduction within a single crystalline framework, offering a versatile platform for the development of intelligent porous materials with real\u2010time visual tracking capabilities.\n                  <\/jats:p>","DOI":"10.1002\/anie.202513288","type":"journal-article","created":{"date-parts":[[2025,7,31]],"date-time":"2025-07-31T10:13:52Z","timestamp":1753956832000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Flexible Hydrogen\u2010Bonded Organic Framework with Anthracene Core for Recognition of Benzene Over Cyclohexane"],"prefix":"10.1002","volume":"64","author":[{"given":"Furong","family":"Yuan","sequence":"first","affiliation":[{"name":"Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 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Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanting","family":"Chen","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenxin","family":"Chen","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gaoyan","family":"Lan","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 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Laboratory of Polymer Materials, College of Chemistry and Materials Science Fujian Normal University  Fuzhou 350000 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