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Here, a breakthrough molecular design strategy employing side\u2010chain\u2010engineered insulating polymers\u2014poly(methyl methacrylate) (PMMA) and poly(benzyl methacrylate) (PBMA)\u2014as multifunctional additives to simultaneously enhance electronic and mechanical properties is presented. Through synergistic control of compatibility, chain diffusivity, and docking position with PM6\/Y6 components, PMMA selectively distributes in the amorphous regions of the PM6 donor while promoting molecular packing in crystalline regions, enabling dual stress\u2010dissipation networks and efficient charge transport pathways. As a result, the rigid 10PMMA (with 10 wt.% PMMA) devices achieve a record 19.01% power conversion efficiency (PCE), while maintaining 18.53% PCE (only 2% loss) for the rigid 20PMMA (with 20 wt.% PMMA) devices. More remarkably, the stretchable 20PMMA devices exhibit exceptional mechanical robustness with 10.8% fracture strain (2.2\u2010fold improvement) and 87% PCE retention after 100 stretching cycles (10% strain), far surpassing the control devices (50% retention). The work establishes fundamental design principles for insulating polymer additives in is\u2010OPVs, demonstrating how molecular control over micro\u2010\/nanoscale distribution can simultaneously optimize electronic and mechanical properties. These findings provide a universal materials platform for high\u2010performance stretchable electronics, particularly for next\u2010generation wearable energy technologies where both efficiency and durability are paramount.<\/jats:p>","DOI":"10.1002\/adma.202510366","type":"journal-article","created":{"date-parts":[[2025,10,28]],"date-time":"2025-10-28T13:41:30Z","timestamp":1761658890000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Side\u2010Chain\u2010Engineered Insulating Polymer Distribution Enables High\u2010performance Intrinsically Stretchable Organic Photovoltaics"],"prefix":"10.1002","volume":"38","author":[{"given":"Shuyang","family":"Sang","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Low\u2010grade Energy Utilization Technologies and Systems School of Energy &amp; Power Engineering Chongqing University  Chongqing 400044 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haozhe","family":"He","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kangkang","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Tianjin Key Laboratory of Molecular Optoelectronic Sciences Key Laboratory of Organic Integrated Circuits Ministry of Education Collaborative Innovation Center of Chemical Science and Engineering Tianjin University  Tianjin 300072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9633-0087","authenticated-orcid":false,"given":"Xiaojun","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaru","family":"Yue","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Low\u2010grade Energy Utilization Technologies and Systems School of Energy &amp; Power Engineering Chongqing University  Chongqing 400044 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zekun","family":"Chen","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingtao","family":"Xiang","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Low\u2010grade Energy Utilization Technologies and Systems School of Energy &amp; Power Engineering Chongqing University  Chongqing 400044 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5407-6209","authenticated-orcid":false,"given":"Bin","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Jiangxi University of Science and Technology  156 Ke Jia Avenue Ganzhou 341000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5884-0083","authenticated-orcid":false,"given":"Long","family":"Ye","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Tianjin Key Laboratory of Molecular Optoelectronic Sciences Key Laboratory of Organic Integrated Circuits Ministry of Education Collaborative Innovation Center of Chemical Science and Engineering Tianjin University  Tianjin 300072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kuan","family":"Sun","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Low\u2010grade Energy Utilization Technologies and Systems School of Energy &amp; Power Engineering Chongqing University  Chongqing 400044 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Changduk","family":"Yang","sequence":"additional","affiliation":[{"name":"School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST)  50 UNIST\u2010gil, Ulju\u2010gun Ulsan 44919 South Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9723-2403","authenticated-orcid":false,"given":"Shanshan","family":"Chen","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Low\u2010grade Energy Utilization Technologies and Systems School of Energy &amp; Power Engineering Chongqing University  Chongqing 400044 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongfang","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,10,28]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-021-03772-0"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-023-06946-0"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aav9653"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/aelm.201800823"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202002529"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aah4496"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2024.08.001"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2025.101851"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-022-01244-y"},{"key":"e_1_2_7_10_1","volume":"64","author":"Wang L.","year":"2025","journal-title":"Adv. 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