Developing high-performance n-type polymer mixed ionic-electronic conductors (PMIECs) is a grand challenge, which largely determines their applications in vaious organic electronic devices, such as organic electrochemical transistors (OECTs) and organic thermoelectrics (OTEs). Herein, two halogen-functionalized PMIECs f-BTI2g-TVTF and f-BTI2g-TVTCl built from fused bithiophene imide dimer (f-BTI2) as the acceptor unit and halogenated thienylene-vinylene-thienylene (TVT) as the donor co-unit are reported. Compared to the control polymer f-BTI2g-TVT, the fluorinated f-BTI2g-TVTF shows lower-positioned lowest unoccupied molecular orbital (LUMO), improved charge transport property, and greater ion uptake capacity. Consequently, f-BTI2g-TVTF delivers a state-of-the-art µC* of 90.2 F cm V s with a remarkable electron mobility of 0.41 cm V s in OECTs and an excellent power factor of 64.2 µW m K in OTEs. An OECT-based inverter amplifier is further demonstrated with voltage gain up to 148 V V , which is among the highest values for OECT inverters. Such results shed light on the impacts of halogen atoms on developing high-performing n-type PMIECs.
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