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However, the ordered crystalline structures required for mechanical performance often sequester ester bonds within crystalline domains, creating an accessibility barrier that hinders chemical recycling and biodegradation. Herein, we decouple this trade\u2010off through a crystallization modulation strategy by incorporating sterically hindered asymmetric pyrrolidone units into the polyester backbone. This molecular engineering approach relocates cleavable ester bonds from crystalline to amorphous domains while preserving semi\u2010crystalline reinforcement, confirmed by x\u2010ray structural analysis. The polymers exhibit tunable mechanical robustness, with tensile strength exceeding 18.7 MPa and lap\u2010shear adhesion up to 15.3 MPa. They undergo complete depolymerization to easily separable soluble oligomers via methanolysis under ambient pressure, even within mixed\u2010plastic streams, enabling closed\u2010loop recycling. Furthermore, the amorphous enrichment of polar units accelerates biodegradation, achieving a mineralization rate 2.3 times that of conventional analogues. This work demonstrates a viable molecular design pathway to reconcile mechanical robustness, mild chemical recyclability, and enhanced environmental degradability in polyethylene\u2010like materials, offering a route to mitigate long\u2010term plastic persistence.<\/jats:p>","DOI":"10.1002\/smll.76266","type":"journal-article","created":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T19:39:34Z","timestamp":1792697974000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mildly Recyclable and Biodegradable Structurally Polyethylene\u2010Like Polyester Enabled by Unlocking Ester Accessibility"],"prefix":"10.1002","author":[{"given":"Hanxu","family":"Zhu","sequence":"first","affiliation":[{"name":"Key Laboratory of Bio\u2010based Polymeric Materials of Zhejiang Province Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo China"},{"name":"University of Chinese Academy of 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