This study aims to investigate the influence of graphene nanoplatelet (GNP) concentration on the electrochemical and tribological properties of GNP-poly(methyl methacrylate) (PMMA) composite coatings. GNP-PMMA coatings were prepared with varying GNP concentrations (0.5, 1.0, 3.0, and 5.0wt %) using the drop-casting method onto AA6061 aluminum alloy substrates. Results showed that the addition of 1.0wt % GNP increased the tensile strength of PMMA but further increase reduced the tensile strength and fracture strain of the composites. Permeability studies indicated that 1.0GNP-PMMA had the lowest water vapour transition rate. All GNP-PMMA coatings showed a higher coating resistance and impedance modulus at the lowest frequency compared to neat PMMA with 1.0GNP-PMMA having the highest |Z|0.01 Hz value in comparison to the composites with higher GNP concentrations. According to Raman mapping, an increase in the concentration of GNP in the composite resulted in the agglomeration of graphene, which caused the debonding of the graphene-PMMA interfaces and also resulted in a higher number of shear fronts and other defects on the fracture surface that reduced barrier properties of graphene. The specific wear rate of 1.0GNP-PMMA was lower than that of neat PMMA, indicating improved wear resistance. The coefficient of friction was lowest for 5.0GNP-PMMA, although this was due to a higher amount of material being transferred to the counterface. Accordingly, optimizing the GNP concentration enables the development of high-performance PMMA coatings with enhanced strength, improved barrier properties, and reduced wear rates, making them well-suited for applications such as corrosion protection and tribological coatings.