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A novel series of naphthalene‐diimide‐based semiconducting polymers (P1–P4) containing benzodithiophene or dithienopyrrole were successfully synthesized for ambipolar semiconducting materials showing near infrared absorptions. The incorporation of a 3‐hexylthiophene (3HT) spacer extended the intramolecular charge‐transfer (ICT) peak from λonset = 739 nm (P1) to 785 nm (P3). Moreover, about 250 nm...