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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]

Flexible organic monitoring system that can work in short‐wave infrared (SIR) region has great potential in autonomous driving, night driving safety, military encryption, biomedical imaging, and robot engineering. Especially, the development of infrared artificial vision system device that can autonomously improve the computing speed and adapt to different brightness ambient light is very important. However, it is a challenge for mimicking infrared visual adaptation because of the need for infrared absorbing materials and the need to control the concentration of carriers. In this study, inorganic quantum dot material is combined with organic materials to promote carrier separation and introduce interface defects that adjust the carrier concentration in transistors, which induce the synaptic behavior under SIR (1100 nm) light in darkness and the ability to adapt to white ambient light. Furthermore, the device array realizes the image recognition of SIR light at night with white ambient light of different brightness, exhibiting good self‐adaptability, and strong anti‐interference ability. These results demonstrate promising applications of the infrared synaptic phototransistors in adapted bionic optoelectronic devices. [ABSTRACT FROM AUTHOR]