In this study, a method for producing nitrogen-modified graphene oxide (NMGO) using hydrothermal synthesis in the presence of triethanolamine is presented. The composition and structure of NMGO are characterized using X-ray phase analysis (XPA), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy, and Raman spectroscopy. Ni-based metal matrix coatings (MMCs) modified with NMGO were obtained from a sulfate-chloride electrolyte in the galvanostatic mode. The process of electrochemical deposition of these coatings was studied using chronovoltammetry. The microstructure of Ni–NMGO MMCs was studied using the XPA and SEM methods. It has been established that the addition of NMGO particles into the Ni matrix results in an increase in the microhardness of the resulting coatings by an average of 1.30 times. This effect is a consequence of the refinement of crystallites and high mechanical properties of NMGO phase. The corrosion-electrochemical behavior of studied electrochemical deposits in 0.5 M sulfuric acid was analyzed. It has been shown that the corrosion rate of Ni–NMGO MMCs in a 3.5% sodium chloride environment decreases by approximately 1.50–1.70 times as compared to unmodified Ni coatings. This is due to NMGO particles that act as a barrier preventing the propagation of the corrosion and form corrosive galvanic microelements with Ni, promoting anodic polarization.