Skin‐Like Soft Thermoelectric Composites with a “J‐Shaped” Stress–Strain Behavior for Self‐Powered Strain Sensing

Abstract Polymer thermoelectric (TE) materials present a promising alternative to actuating low‐power wearable electronics without an additional power source, among which poly(3,4‐ethylenedioxythiophene) (PEDOT):poly(styrenesulfonate) (PSS) is a promising candidate. However, it is too hard and brittle to integrate into wearables seamlessly and comfortably. Herein, PEDOT:PSS‐based TE composites with simultaneous softness and stretchability are fabricated by a water‐borne polyurethane (WPU) and PEDOT:PSS mixture containing the judiciously chosen ionic liquid (IL) and subsequent drop casting. The obtained composites show a stable TE voltage, high stretchability (>500%), ultra‐flexibility, and excellent sensitivity (gauge factor = 1251). More importantly, it exhibited “J‐shaped” stress–strain curves resembling human skins after a loading/releasing treatment. The skin‐like nonlinear elastic behavior combines enough softness in the “toe” region, high stretchability, and a strong strain hardening at the late deformation stage, enabling its seamless and comfortable integration with the human body. Given the desired mechanical performance and strain‐sensing capability, the composite is designed to serve as a self‐powered sensor with high sensitivity and accuracy, suggesting a high potential in human motion detection. This work demonstrates the versatility of the developed skin‐like PEDOT:PSS‐based composites in wearable electronics.