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However, progress in this field remains limited by underdeveloped design principles, and the development of ambipolar single\u2010component organic mixed ionic\u2010electronic conductors (OMIECs) has lagged significantly. Herein, we design a novel electron\u2010deficient building block\n                    <jats:bold>BITBII<\/jats:bold>\n                    , and copolymerize it with distinct electron\u2010donating units to obtain two polymers (\n                    <jats:bold>PBITBII\u20102FT, PBITBII\u2010F2T<\/jats:bold>\n                    ). PBITBII\u2010F2T\u2010based single\u2010component OECTs exhibited excellent ambipolar performance (p\u2010type\/n\u2010type normalized transconductances (g\n                    <jats:sub>m, norm<\/jats:sub>\n                    ): 4.7\/2.92 S cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    ;\n                    <jats:italic>\u00b5<\/jats:italic>\n                    C\n                    <jats:sup>*<\/jats:sup>\n                    : 63.37\/14.58 F V\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    s\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    ). In contrast,\n                    <jats:bold>PBITBII\u20102FT<\/jats:bold>\n                    exhibited only relatively weak n\u2010type characteristics. Through theoretical calculations and film morphology analysis, the loss of ambipolarity in\n                    <jats:bold>PBITBII\u20102FT<\/jats:bold>\n                    is attributed to a more localized HOMO distribution, a wavy backbone leading to inferior intermolecular packing, and a rougher film morphology, all of which impede hole transport. Furthermore, a complementary inverter fabricated using\n                    <jats:bold>PBITBII\u2010F2T<\/jats:bold>\n                    achieves a high voltage gain of up to 29.1\u00a0V\/V. Cytotoxicity tests confirm the good biocompatibility of\n                    <jats:bold>PBITBII\u2010F2T<\/jats:bold>\n                    . This work not only enriches the material library for high\u2010performance ambipolar OECTs but also provides valuable insights into structure\u2013property relationships governing ambipolar functionalities, offering guidance for future ambipolar molecular engineering.\n                  <\/jats:p>","DOI":"10.1002\/smll.73556","type":"journal-article","created":{"date-parts":[[2026,4,28]],"date-time":"2026-04-28T08:35:22Z","timestamp":1777365322000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Switching N\u2010Type to Ambipolar Organic Electrochemical Transistors by Donor Engineering of Polymeric Mixed Conductors Based on a Novel Electron\u2010Deficient BITBII Building Block"],"prefix":"10.1002","volume":"22","author":[{"given":"Chong","family":"Ran","sequence":"first","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongsheng","family":"Yu","sequence":"additional","affiliation":[{"name":"Central Laboratory The Third Affiliated Hospital of Sun Yat\u2010Sen University Yuedong Hospital  Meizhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Biao","family":"Peng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayao","family":"Duan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiuyuan","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juntao","family":"Tan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxiong","family":"Tian","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhengke","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Optoelectronic Materials and Technologies Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, School of Materials Science and Engineering Sun Yat\u2010sen University  Guangzhou P. R. 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