The coating of magnesia partially stabilized zirconia (Mg-PSZ) with a bioactive glass was investigated for enhancing the bioactivity and bone-bonding ability of Mg-PSZ orthopedic implants. Individual coatings of three different bioactive glasses were prepared by depositing a concentrated suspension of the glass particles on Mg-PSZ substrates, followed by sintering at temperatures between 750 °C and 850 °C. Two silicate-based glass compositions (designated 13–93 and 6P68), and a borosilicate glass composition (H12) were investigated. The microstructure and adhesive strength of the coatings were characterized, and the in vitro bioactivity of the glasses was compared by measuring their conversion kinetics to hydroxyapatite in an aqueous phosphate solution at 37 °C. The 6P68 glass provided the highest adhesive strength (40 ± 2 MPa) but showed very limited bioactivity, whereas the H12 glass had lower adhesive strength (18 ± 2 MPa) but the highest bioactivity. A functionally graded coating, consisting of a 6P68 interfacial layer and an H12 surface layer, was developed to provide a coating with high adhesive strength coupled with rapid in vitro bioactivity.