HighlightsConstruction of a viscoelastic composite nacre with a ripple-like layered architecture through supramolecular interactions.Outstanding self-adhesion, self-healing and scrape-resistant mechanical and thermal properties.Utility as an integrated heat spreader and TIMs for “chameleon-like” thermal management of planar soft electronics.Supplementary InformationThe online version contains supplementary material available at 10.1007/s40820-023-01149-8.