Super Tough and Spontaneous Water‐Assisted Autonomous Self‐Healing Elastomer for Underwater Wearable Electronics

Abstract Self‐healing soft electronic material composition is crucial to sustain the device long‐term durability. The fabrication of self‐healing soft electronics exposed to high moisture environment is a significant challenge that has yet to be fully achieved. This paper presents the novel concept of a water‐assisted room‐temperature autonomous self‐healing mechanism based on synergistically dynamic covalent Schiff‐based imine bonds with hydrogen bonds. The supramolecular water‐assisted self‐healing polymer (WASHP) films possess rapid self‐healing kinetic behavior and high stretchability due to a reversible dissociation–association process. In comparison with the pristine room‐temperature self‐healing polymer, the WASHP demonstrates favorable mechanical performance at room temperature and a short self‐healing time of 1 h; furthermore, it achieves a tensile strain of 9050%, self‐healing efficiency of 95%, and toughness of 144.2 MJ m−3. As a proof of concept, a versatile WASHP‐based light‐emitting touch‐responsive device (WASHP‐LETD) and perovskite quantum dot (PeQD)‐based white LED backlight are designed. The WASHP‐LETD has favorable mechanical deformation performance under pressure, bending, and strain, whereas the WASHP‐PeQDs exhibit outstanding long‐term stability even over a period exceeding one year in a boiling water environment. This paper provides a mechanically robust approach for producing eco‐friendly, economical, and waterproof e‐skin device components.