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Alumina (Al2O3) thin film coatings are applied on Al alloys using Plasma Electrolytic Oxidation (PEO) method to reduce the wear and corrosion problems. Plasma Electrolytic Aluminating (PEA) is a technique which could generate Alumina coatings on cast iron, mild steel and copper alloys. In this study, the aim is to explore the anti-wear and anti-corrosion behaviours of PEA Alumina coatings on gray cast iron. The dry sliding tribology test data was obtained from Pin-on-Disk (POD) tests against SAE 52100 steel and Tungsten Carbide (WC) counterfaces. Comparing with the PEO Alumina coatings, the PEA Alumina coating has much lower Coefficient of Friction (COF) and less wear. The microstructure, chemical composition and phase composition of this coating were investigated with Scanning Electron Microscope (SEM), Energy-Dispersive X-Ray Spectroscopy (EDX) and X-Ray Diffraction (XRD), respectively. There was FeO (or FeAl2O4) found on the PEA Alumina coating.