 Strong self-healing materials with high healing efficiency are of great use in many fields, but their fabrication is extremely challenging. Here, the authors present a robust self-healing material by incorporating high-density non-covalent bonds at the interfaces between dendritic tannic acid-modified tungsten-dissulfide nano-sheets and a polyurethane matrix to collectively produce a strong interfacial interaction. This article was authored by Yi'en Wang, Xinhuang, and Xinxing Zhong.