In this study, acrylic-epoxy-based nanocomposite coatings loaded with different concentrations (0.5–3 wt.%) of graphene oxide (GO) nanoparticles were successfully prepared via the solution intercalation approach. The thermogravimetric analysis (TGA) revealed that the inclusion of GO nanoparticles into the polymer matrix increased the thermal stability of the coatings. The degree of transparency evaluated by the ultraviolet–visible (UV–Vis) spectroscopy showed that the lowest loading rate of GO (0.5 wt.%) had completely blocked the incoming irradiation, thus resulting in zero percent transmittance. Furthermore, the water contact angle (WCA) measurements revealed that the incorporation of GO nanoparticles and PDMS into the polymer matrix had remarkably enhanced the surface hydrophobicity, exhibiting the highest WCA of 87.55º. In addition, the cross-hatch test (CHT) showed that all the hybrid coatings exhibited excellent surface adhesion behaviour, receiving 4B and 5B ratings respectively. Moreover, the field emission scanning electron microscopy (FESEM) micrographs confirmed that the presence of the functional groups on the GO surface facilitated the chemical functionalization process, which led to excellent dispersibility. The GO composition up to 2 wt.% showed excellent dispersion and uniform distribution of the GO nanoparticles within the polymer matrix. Therefore, the unique features of graphene and its derivatives have emerged as a new class of nanofillers/inhibitors for corrosion protection applications.