Wearable electronics have significantly advanced the development of highly stretchable strain sensors, which are essential for applications such as health monitoring, human-machine interfaces, and energy harvesting. Fiber-based sensors and polymeric materials are promising due to their flexibility and tunable properties, although balancing sensitivity and stretchability remains a challenge. This study introduces a novel composite strain sensor that combines poly(3-hexylthiophene) and tetrafluoro-tetracyanoquinodimethane to form a charge-transfer complex (CTC) with carbon nanotubes (CNTs) on a styrene-butadiene-styrene substrate. The CTC improves conductivity through effective charge transfer, while CNTs provide mechanical reinforcement and maintain conductive paths, preventing cracks under large strains. Purposefully introduced wrinkles in the structure enhance the detection of small strains. The sensor demonstrated a broad strain-sensing range from 0.01 to 200%, exhibiting high sensitivity to both minor and major deformations. Mechanical tests confirmed strong stress-strain performance, and electrical tests indicated significant conductivity improvements with CNT integration. These results highlight the potential of the sensor for applications in health monitoring, human-machine interfaces, and energy harvesting, effectively mimicking the tactile sensing abilities of human skin.
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