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.