In the present work, the corrosion properties and the surface chemistry of a graphene oxide-coated AZ91D alloy were investigated. The coatings were deposited on the substrate specimens by immersion in solutions with GO concentrations of 0.05% and 0.1% (m/v). An intermediate silane layer was firstly obtained to improve adhesion between the GO films and the AZ91D substrate. The electrochemical behavior of the coated specimens was assessed using electrochemical impedance spectroscopy and potentiodynamic polarization curves in 3.5 wt.% NaCl solution. The surface chemistry was assessed using X-ray photoelectron spectroscopy (XPS). The GO films consisted of a mixture of carbon-based bonds (C-C, C-OH, C=O, and O-C=O). The surface morphology of the coated specimens was examined using scanning electron microscopy. The results revealed that the compactness of the GO films was dependent on the deposition conditions. The corrosion resistance was affected by the surface morphology.