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Here, we report a molecular-level strategy to enhance PEDOT:PSS films via electron-withdrawing substituents in benzoic acid. Fluoro (\u2013F) and cyano (\u2013CN) groups synergistically tune chain conformation, molecular ordering, and carrier-state distribution. Furthermore, the cyano and fluoro groups introduce energy barriers that selectively filter low-energy carriers, thereby reducing bipolaron content and boosting the Seebeck coefficient, while facilitating PSS removal and improving electrical conductivity. The optimized DMSO:2-fluoro-5-cyanobenzoic acid (DMSO:2F5CBA) treated film exhibits a conductivity of &amp;gt;1200 S cm\u20131, a Seebeck coefficient of 43.8 \u03bcV K\u20131, and a power factor of 188.89 \u03bcW m\u20131 K\u20132. Spectroscopic and morphological analyses confirm effective modulation of carrier states, chain ordering, and phase separation. This work demonstrates a multifaceted approach where energy filtering and structural optimization synergistically enhance thermoelectric performance, providing a promising route toward high-performance flexible organic thermoelectrics.<\/jats:p>","DOI":"10.1021\/acsami.6c17862","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T07:01:20Z","timestamp":1790838080000},"page":"55546-55558","source":"Crossref","is-referenced-by-count":0,"title":["Multifaceted Tuning of PEDOT:PSS with Electron-Withdrawing Effect for Superior Thermoelectric Performance"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-0682-414X","authenticated-orcid":true,"given":"Zishun","family":"Zhou","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiajun","family":"Wang","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingjie","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dingshuai","family":"Hou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxiang","family":"Pei","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chumeng","family":"Xiang","sequence":"additional","affiliation":[{"name":"Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongbo","family":"Fan","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University , , Hung Hom , ,","place":["Hong Kong, P.R. China, 100872"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0164-9322","authenticated-orcid":true,"given":"Weijia","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. China, 710072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1405-9279","authenticated-orcid":true,"given":"Huiqing","family":"Fan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Northwestern Polytechnical University , , ,","place":["Xi'an, P.R. 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