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However, integrating high mechanical robustness, versatile shape programmability, and excellent printability into a single material system remains challenging. Here, an orthogonal photochemistry\u2010confined crystallization strategy is developed to fabricate mechanically robust, printable shape\u2010programmable polymers. This approach utilizes a rationally designed photochemical process to trigger radical polymerization and phenol coupling synchronously yet orthogonally, enabling one\u2010step formation of a covalent double\u2010network that efficiently confines polymer crystallization during solvent evaporation. The resulting homogeneous, refined crystalline domains greatly enhance stretchability (1891%) and toughness (41\u00a0MJ m\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>3<\/jats:sup>\n                    ) by up to 63\u2010 and 103\u2010fold, respectively, compared to counterparts lacking network confinement, while also maintaining fatigue resistance over 1500 stretching cycles. The synergy between confined crystallization and double\u2010network confinement further confers shape reconfiguration and shape\u2011memory morphing, affording robust shape programmability under thermal stimuli. Moreover, the efficient photo\u2011mediated gelation, coupled with solvent evaporation, enables rapid and controllable solidification fully compatible with additive manufacturing. Leveraging these capabilities, and as a proof\u2010of\u2010concept, the developed polymers are printed and assembled into bioinspired soft actuators capable of integrated active actuation and precise sensing. This work provides new insight into the photochemical design of high\u2010performance shape\u2010programmable polymers and advanced soft devices.\n                  <\/jats:p>","DOI":"10.1002\/anie.7052006","type":"journal-article","created":{"date-parts":[[2026,8,29]],"date-time":"2026-08-29T05:37:05Z","timestamp":1787981825000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Orthogonal Photochemistry\u2010Confined Crystallization Enables Mechanically Robust, Printable Shape\u2010Programmable Polymers"],"prefix":"10.1002","volume":"65","author":[{"given":"Beijia","family":"Yuan","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Science Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education Northwest University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tong","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education Northwest University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanpei","family":"Tian","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education Northwest University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yulin","family":"Xiong","sequence":"additional","affiliation":[{"name":"School of Astronautics Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhe","family":"Lu","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education Northwest University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9911-8452","authenticated-orcid":false,"given":"Ming","family":"Lei","sequence":"additional","affiliation":[{"name":"School of Astronautics Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6653-7594","authenticated-orcid":false,"given":"Zijian","family":"Zheng","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology Faculty of Science The Hong Kong Polytechnic University  Hong Kong SAR P.R. 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