The reinforcing effect of graphene oxide (GO) and its derivatives for polymer matrices highly depends on their dispersion therein. Thus, a facile method was developed to enhance the dispersibility of GO via compounding with -methacryloxypropyltrimethoxysilane (GO-KH570). The interfacial interactions between GO and KH570, as well as the surface morphology, chemical composition and polarity, were investigated by molecular dynamics simulation combined with experimental methods. Findings indicate that KH570 can successfully graft onto the surface of GO nanosheets via the covalent bonding, and the polarity of the as-obtained GO-KH570 can be tuned by adjusting the dosage of KH570. Besides, the GO-KH570 was further used as the filler to improve performances of polyimide (PI) matrix. After using this GO-KH570 composite, the PI-based coating was endowed with excellent wear resistance and corrosion resistance properties. Particularly, PI/GO-KH570-2 coating with a GO-KH570-2 dosage of 0.5wt% exhibits much higher hardness, showing promising potential as the candidate high-performance coating in aerospace and marine industries.