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Abstract: Thiazoloisoindigo, a novel structural variation of isoindigo, is for the first time utilized to synthesize conjugated polymers. The polymer based on thiazoloisoindigo merges the advantages of the one based on thienoisoindigo and diazaisoindigo; it not only exhibits a greatly redshifted UV/Vis absorption to the near‐infrared region owing to its strong tendency to form quinoidal structures, similar to that based on thienoisoindigo, but also shows excellent ambipolar mobility (hole: 3.93, electron: 1.07 cm2 V−1 s−1) in organic field‐effect transistors (OFETs), superior to that based on diazaisoindigo, showing the strong electron‐withdrawing capability of thiazoloisoindigo. [ABSTRACT FROM AUTHOR]