Bioactive Plasma Electrolytic Oxidation (PEO) coatings enriched in Ca, P and F were developed on Mg0.6Ca and Mg0.6Ca2Ag alloys with the aim to impede their fast degradation rate. Different characterization techniques (SEM, TEM, EDX, SKPFM, XRD) were used to analyze the surface characteristics and chemical composition of the bulk and/or coated materials. The corrosion behaviour was evaluated using hydrogen evolution measurements in Simulated Body Fluid (SBF) at 37 °C for up to 60 days of immersion. PEO-coated Mg0.6Ca showed a 2–3-fold improved corrosion resistance compared with the bulk alloy, which was more relevant to the initial 4 weeks of the degradation process. In the case of the Mg0.6Ag2Ag alloy, the obtained corrosion rates were very high for both non-coated and PEO-coated specimens, which would compromise their application as resorbable implants. The amount of F− ions released from PEO-coated Mg0.6Ca during 24 h of immersion in 0.9% NaCl was also measured due to the importance of F− in antibacterial processes, yielding 33.7 μg/cm2, which is well within the daily recommended limit of F− consumption.