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Despite their desirable stretchability and self\u2010healing, inherent limitations in dielectric polarization and interfacial modulation restrict optoelectronic performance, creating an unresolved trade\u2010off between functionality and sustainability. Guided by green chemical engineering and circular economy principles, we designed a degradable polycarbonate\u2010based thermoplastic polyurethane (PCTPU) by incorporating PC soft segments into the polyurethane backbone, and constructed a robust non\u2010covalent hydrogen\u2010bonding network via poly (amic acid) (PAA) blending to synergistically regulate dielectric polarization and interfacial compatibility. The PCTPU\u2013PAA composite exhibits excellent mechanical performance and enhanced self\u2010healing property. Notably, when integrated into organic neuromorphic visual sensors (ONeuVS), the composite enables a \u223c7.6\u2010fold enhancement in carrier mobility versus bare PCTPU sensors. 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This work establishes a scalable molecular engineering strategy for high\u2010performance, sustainable flexible dielectrics and devices, breaking the performance\u2013sustainability trade\u2010off and facilitating their large\u2010scale green applications.<\/jats:p>","DOI":"10.1002\/adma.74824","type":"journal-article","created":{"date-parts":[[2026,8,27]],"date-time":"2026-08-27T09:55:01Z","timestamp":1787824501000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecularly Engineered Degradable PCTPU\u2013PAA Dielectrics With Boosted Carrier Mobility for Retina\u2010Mimic Neuromorphic Visual Sensors Toward Closed\u2010Loop Green Flexible Electronics"],"prefix":"10.1002","volume":"38","author":[{"given":"Zijie","family":"Yang","sequence":"first","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin 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