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Shape recovery inevitably leads to a dramatic decrease of Young's modulus due to the enhanced flexibility of polymer chains at the transition temperature. Herein, the principle of phase\u2010transition\u2010induced stiffening of shape\u2010memory metallic alloys (SMAs) is introduced to the design of molecular structures for shape\u2010memory polyurethane (SMPUs), featuring all\u2010hard segments composed of main chains that are attached with poly(ethylene glycol) (PEG) dangling side chains. Different from conventional SMPs, they achieve a soft\u2010to\u2010stiff transition when shape recovers. The stiffening process is driven by water\u2010triggered segmental rearrangement due to the incompatibility between the hard segments and the soft PEG segments. Upon hydration, the extent of microphase separation is enhanced and the hard domains are transformed to a more continuous morphology to realize more effective stress transfer. Meanwhile, such segmental rearrangement facilitates the shape\u2010recovery process in the hydrated state despite the final increased glass transition temperature (<jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub>). This work represents a novel paradigm of simultaneously integrating balanced mechanics, shape\u2010memory property, and biocompatibility for SMPUs as materials for minimally invasive surgery such as endoluminal stents.<\/jats:p>","DOI":"10.1002\/adma.202201914","type":"journal-article","created":{"date-parts":[[2022,5,3]],"date-time":"2022-05-03T02:28:45Z","timestamp":1651544925000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":87,"title":["Water\u2010Triggered Stiffening of Shape\u2010Memory Polyurethanes Composed of Hard Backbone Dangling PEG Soft Segments"],"prefix":"10.1002","volume":"34","author":[{"given":"Wenkai","family":"Liu","sequence":"first","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Med\u2010X Center of Materials Sichuan University  Chengdu 610065 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