In this paper, the graphene oxide loaded with nano titanium dioxide (TiO2–GO) was synthesized through 3-isocyanatopropyltrimethoxysilane (IPTMS) and characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction analysis (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and dispersion test. The results illustrated our modification was successful and TiO2–GO was transferred from hydrophilic to hydrophobic. That greatly enhanced the dispersity of TiO2–GO in epoxy through the observation of the coating morphology test. Moreover, the impact of TiO2–GO on anti-corrosion property in epoxy was investigated by Electrochemical Impedance Spectroscopy (EIS). Comparing to pristine particles including GO and TiO2, TiO2–GO could more significantly improve the resistance of corrosion with the help of IPTMS. Furthermore, the anti-corrosion mechanism of TiO2–GO in epoxy was tentatively proposed and discussed.