This study discusses the synthesis, characterization and development of self-healing nanocomposite of amino-terminated PDMS (Polydimethylsiloxane), Epoxy (EPON828¸ Diethylenetriamine (DETA)), and Graphene Oxide (GO).GOwas prepared using a modified Hummer’s method andwas incorporated into the PDMS-Epoxy composite in various ratios (0.1 wt.%, 0.3 wt.%, and 0.5 wt.%) using toluene as the dispersing medium. Fourier TransformInfrared Spectroscopy was used for confirming the presence of the designed/prepared structures, and thermo-mechanical analysis was performed to test the change in glass transition temperature and initiation temperature of self-healing process. The composite resins were coated on mild steel substrates by curing freshly prepared resins over the substrates at elevated temperatures. The corrosion behavior of mild steel in 3.5 wt.% NaCl solution before and after the coatings was studied using Tafel Electrochemical Polarization test. The self-healing properties of the materials were also studied by applying cuts on the material and letting them heal under elevated temperatures, and the results showed that the prepared coating demonstrated an effective corrosion resistance for mild steel for various marine applications.