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Stretchable electrodes are critical to the development of advanced technologies such as human–machine interaction, flexible sensing, and wearable power supply, making them of significant research value. However, the current preparation methods for high‐performance stretchable electrodes are complex and inefficient, posing challenges for their large‐scale application in the realm of flexible wearables. To address this need, a straightforward and efficient embedding strategy is reported for fabricating stretchable silver nanowire/thermoplastic elastomer composite electrodes (referred to as Strem‐AT) utilizing the viscoelasticity and outstanding mechanical properties of polymer elastomers to achieve outstanding extensibility, conductivity, and a smooth surface. These electrodes exhibit excellent tensile behavior, low surface roughness, and stable electrical properties, enabling their successful integration into stretchable sensors and intrinsically stretchable organic photovoltaic cells (IS‐OPV). When applied to human skin joints for motion detection, the sensor demonstrates remarkable stretchability and stable signal output. Importantly, the all‐polymer IS‐OPV exhibits a top‐notch power conversion efficiency (PCE) of >12.5% and a PCE80% strain exceeding 50%. Furthermore, even after subjecting high‐strain stretching at 50% for 1000 cycles, the IS‐OPV can retain 76% of the initial PCE. This study presents a multifunctional stretchable electrode with high repeatability and easy‐to‐scale fabrication in wearable sensors and photovoltaics. [ABSTRACT FROM AUTHOR]

Intrinsically stretchable organic photovoltaic cells (OPVs) have garnered significant attention as crucial devices for powering next‐generation wearable electronics. Despite the rapid power conversion efficiency gains in champion OPVs, their brittle stretchability has failed to meet the demands of the Internet of Things era, severely hindering further development and practical applications. In this regard, a new dual‐donor polymer blending strategy is demonstrated for constructing intrinsically stretchable OPVs by designing a novel high‐molecular–weight conjugated polymer PM6‐HD. This PM6 derivative featuring long alkyl chains can reach a sufficiently high molecular weight and thus exhibits a high fracture strain exceeding 90%, which is ≈12 times higher than the benchmark PM6. Synergistic optimization of mechanical properties and photovoltaic performance in polymer:small molecule and all‐polymer systems constructed from the physical blends of PM6 and PM6‐HD is achieved. Crucially, the resulting intrinsically stretchable OPV demonstrates excellent stretchability and stability, with a record PCE80% strain of 50.3% and the efficiency retention of above 80% even after 1000 cycles of cyclic stretching at high strains. This work contributes to the advancement of intrinsically stretchable OPV technology and opens up new possibilities for its integration into wearable electronic devices. [ABSTRACT FROM AUTHOR]