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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]

This article discusses the recent progress in the development of high-mobility polymer semiconductors with various functionalities. These semiconductors have advantages such as easy solution processing, large-area manufacturing, mechanical strength, and flexibility. The article focuses on the integration of high mobility with stretchability, strong luminescence, photolithography patterning, and efficient thermoelectric conversion. The challenges and future directions in this field are also discussed. The research is supported by various funding sources. [Extracted from the article]