Phosphate and aluminate electrolytes were used to prepare plasma electrolytic oxidation (PEO) coatings on 6061 aluminum alloy. The surface and cross-section microstructure, element distribution, and phase composition of the PEO coatings were characterized by SEM, EDS, XPS, and XRD. The friction and wear properties were evaluated by pin-on-disk sliding tests under dry conditions. The corrosion resistance of PEO coatings was investigated by electrochemical corrosion and salt spray tests in acidic environments. It was found that the PEO coatings prepared from both phosphate and aluminate electrolytes were mainly composed of α-Al₂O₃ and γ-Al₂O₃. The results demonstrate that a bi-layer coating is formed in the phosphate electrolyte, and a single-layered dense alumina coating with a hardness of 1300 HV is realizable in the aluminate electrolyte. The aluminate PEO coating had a lower wear rate than the phosphate PEO coating. However, the phosphate PEO coating showed a better corrosion resistance in acidic environment, which is mainly attributed to the presence of an amorphous P element at the substrate/coating interface.