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Intrinsically stretchable light‐emitting polymer semiconductors are essential building blocks for bioelectronics and display textiles. Stretchability is challenging for rigid conjugated polymers unless sacrificing charge mobility by introducing amorphous domains. High‐performance light‐emitting properties designed with twisted angle are undesirable for conductive materials. Hence, the concurrent strategies hardly satisfy the balance of stretchability, light‐emitting and mobility. Herein, a morphology engineering is proposed by controlling micro‐crystalline and limiting aggregation, that four intrinsically stretchable emissive polymers with good charge mobility based on indacenodithiophene (IDT) are obtained. Polymers reveal good emission properties with high photoluminescence quantum yields (PLQY) of about 20%, while stretchable modulus and charge mobility are tunable by backbone and weight. Specifically emphasizing, IDT‐2T‐H retains high performance of charge mobility and PLQY even at 100% strain. Therefore, organic light emitting diodes are fabricated based on it and showing the luminance of 176.2 cd cm−2, which verifies the potential of technique to reconcile integration of stretchability, light‐emitting, and mobility. This is the first attempt to integrate balanced mechanical, optical, and electrical properties through micro‐crystalline aggregation‐limited morphology in one polymer, offering a feasible approach to advanced integrated circuit and multi‐functional electronics in the future. [ABSTRACT FROM AUTHOR]

For donor–acceptor conjugated polymers, it is an effective strategy to improve their electron mobilities by introducing electron‐withdrawing groups (EWGs, such as F, Cl, or CF3) into the polymer backbone. However, the introduction of different EWGs always requires a different synthetic approach, leading to additional arduous work. Here, an effective two‐step method is developed to obtain EWG substituted bay‐annulated indigo (BAI) units. This method is effective to introduce various EWGs (F, Cl, or CF3) into BAI at different substituted positions. Based on this method, EWG substituted BAI acceptors, including 2FBAI, 2ClBAI, and 2CF3BAI, are reported for the first time. Furthermore, four polymers of PBAI‐V, P2FBAI‐V, P2ClBAI‐V, and P4OBAI‐V are developed. All the polymers show ambipolar transport properties. Particularly, P2ClBAI‐V exhibits remarkable hole and electron mobilities of 4.04 and 1.46 cm2 V−1 s−1, respectively. These mobilities are among the highest values for BAI‐based polymers. Here, an effective two‐step method is developed to obtain an electron‐withdrawing group (EWG) substituted bay‐annulated indigo (BAI) units. Four polymers, PBAI‐V, P2FBAI‐V, P2ClBAI‐V, and P4OBAI‐V, are developed by this method. Particularly, P2ClBAI‐V exhibits remarkable hole and electron mobilities of 4.04 and 1.46 cm2 V−1 s−1, respectively. These mobilities are among the highest values for BAI‐based polymers. [ABSTRACT FROM AUTHOR]