A Liquid Metal Joule Heater‐Assisted, Rapidly Self‐Healing Dual‐Mode Sensor Based on a Vitrimer‐Like Elastomer for Biosignal Monitoring

ABSTRACT Currently reported wearable sensors based on soft polymeric materials are vulnerable to mechanical damage but rarely achieve rapid repair, reliable multimodal readout, and low crosstalk. We report a fully self‐healing dual‐mode sensor patch based on newly synthesized vitrimer‐like self‐healing elastomer (V‐SHE) with an integrated liquid metal Joule heater. V‐SHE enables rapid self‐healing via thermal heating at near body temperature of 40°C in 30 min, owing to incorporation of both associative and dissociative dynamic bonds into the hydrogen bond‐rich polymer backbone and further reinforcement with an epoxide crosslinker. A dual‐mode sensor fabricated with PEDOT:PSS/CNT coated microporous V‐SHE foam allows recovery of performance over repetitive cycles of cut/ thermal healing as well as interference‐free, simultaneous pressure and temperature sensing, with self‐powered operation via Seebeck transduction. Furthermore, on‐demand much faster self‐healing within 5 min is enabled by the liquid metal‐based Joule heater. This work demonstrates the potential application of our fast self‐healing dual‐mode sensor with a Joule heater to future highly durable and deformable electronics with longevity.