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While material innovation and structural designs have advanced stretchability, a fundamental trade-off often persists between charge transport and elastic deformation. Side-chain engineering emerges as a precise molecular design strategy to transcend this compromise. By decorating conjugated polymer backbones with tailored functional groups, it is possible to intrinsically engineer intermolecular interactions, packing morphology, and energy dissipation mechanisms, thereby synergistically enhancing conductivity, stretchability, and even introducing other functions like self-healing. This review systematically examines this paradigm from a functional-group-centric perspective. We first categorize and elucidate the mechanisms of key side-chain groups\u2014alkyl, hybrid, oligoether, fluoroalkyl, composite, and special functional groups\u2014in regulating the mechanical-electronic property nexus. Subsequently, we critically analyze the application of these engineered materials in advanced functional devices, including skin-conformal sensors, stretchable displays and photodetectors, and neuromorphic computing circuits. Finally, we provide forward-looking perspectives on the challenges and opportunities in designing next-generation side-chains for multifunctional, reliable, and commercially viable stretchable electronics.<\/jats:p>","DOI":"10.1021\/acsami.6c05140","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T20:01:50Z","timestamp":1786564910000},"page":"44671-44699","source":"Crossref","is-referenced-by-count":1,"title":["Enhancing Stretchability and Function in OFETs: A Molecular Design Paradigm via Side-Chain Engineering"],"prefix":"10.1021","volume":"18","author":[{"given":"Hongyang","family":"Wang","sequence":"first","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-3302-8244","authenticated-orcid":true,"given":"Yuzhe","family":"Gu","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]},{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaotian","family":"Wang","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]},{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenqiong","family":"Fan","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Benfei","family":"Xu","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7252-854X","authenticated-orcid":true,"given":"Yang","family":"Li","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]},{"name":"Nanjing University of Posts & Telecommunications (NJUPT) , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"issue":"7994","key":"2026091814063503500_cit1","doi-asserted-by":"publisher","first-page":"276","DOI":"10.1038\/s41586-023-06860-5","article-title":"Three-dimensional integration of two-dimensional field-effect transistors","volume":"625","author":"Jayachandran","year":"2024","journal-title":"Nature"},{"issue":"9","key":"2026091814063503500_cit2","doi-asserted-by":"publisher","first-page":"1078","DOI":"10.1038\/s41563-023-01626-w","article-title":"Scalable integration of hybrid high-\u03ba dielectric materials on two-dimensional semiconductors","volume":"22","author":"Xu","year":"2023","journal-title":"Nat. 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