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With increasing demand for scratch-resistant flexible electronics, the development of transparent coatings with good scratch resistance and self-healing properties has emerged as a key research topic. In this study, a high-strength self-healing poly(urethane – urea) (PUU)-based nanocomposite coating was prepared by introducing functionalized nanodiamond (ND) into a PUU matrix via solution blending. The PUU matrix had hard-segment repeating units and was constructed using isophorone diamine and isophorone isocyanate. The ND particles were modified using a silane coupling agent, 3-aminopropyltriethoxysilane, to obtain well-dispersed KH-ND nanoparticles. KH-ND promoted microphase separation in the PU matrix, inducing the formation of dense and homogeneous hard domains that dissipated stress, prevented further crack development, and improved the mechanical properties and scratch resistance of the coating. In addition, the coating exhibited excellent self-healing properties. Fourier-transform infrared spectroscopy, scanning electron microscopy, and atomic force microscopy were used to characterize the self-healing and hardening mechanisms of the coating. The environmentally friendly PUU/KH-ND coating is easy to prepare and has broad application prospects in transparent and anti-scratch coatings for flexible electronics, automobiles, and home appliances. [ABSTRACT FROM AUTHOR]