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This study proposes a molecular level design strategy for side\u2010chain azobenzene\u2010containing semicrystalline polymers that demonstrate exceptional intrinsic thermal conductivity with photoresponsive actuation and recyclability. By precisely regulating the spatial distribution and content of azobenzene groups and hydrogen\u2010bond network along the polymer chain through controlled radical polymerization, a thermal conduction network featuring \u201chigh\u2010efficiency conduction within crystal domains and low\u2010resistance interfacial connections\u201d was constructed. Azobenzene moieties self\u2010assemble into highly oriented crystalline domains through \u03c0\u2013\u03c0 stacking, where their dense packing significantly enhances phonon coupling efficiency and increases phonon mean free paths. Concurrently, the dynamic reversibility of hydrogen bonds guides domain\u2010boundary molecular chains to form gradual phase transitions, suppressing phonon scattering at amorphous\u2010crystalline interfaces and improving phonon transport efficiency. The film of random copolymer with 35 azobenzene units achieves an outstanding highest intrinsic\n                    <jats:italic>\u03bb<\/jats:italic>\n                    of 2.01\u00a0W\/(m\u00b7K), representing a substantial improvement over its block copolymer counterpart (with a higher crystallinity) and traditional polymers. Additionally, the photoisomerization property of azobenzene endows the material with light\u2010controlled dynamic deformation capabilities. Meanwhile, the noncrosslinked polymer films feature easy recyclability\/reprocessability.\n                  <\/jats:p>","DOI":"10.1002\/anie.202512721","type":"journal-article","created":{"date-parts":[[2025,8,1]],"date-time":"2025-08-01T06:18:51Z","timestamp":1754029131000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["Recyclable Side\u2010Chain Azobenzene\u2010Based Semicrystalline Polymer Films with Outstanding Intrinsic Thermal Conductivity and Photoresponsive Actuation"],"prefix":"10.1002","volume":"64","author":[{"given":"Qingqing","family":"Kong","sequence":"first","affiliation":[{"name":"Shaanxi Key Laboratory of Macromolecular Science and Technology, School of Chemistry and Chemical Engineering Northwestern Polytechnical University  Xi'an Shaanxi 710072 P.R. 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