It is believed that magnesium and its alloys may find applications in biomedical fields as implants, bone fixation devices, and tissue engineering scaffolds. However, their corrosion rate must be controlled. In this study, biomedical magnesium-calcium (Mg-Ca) alloys were ion-implanted with zinc. The surface nanomechanical performance and corrosion behavior of the ion-implanted Mg-Ca alloys are determined. The results show that zinc ion implantation at a dose of 0.9×10 17 ions/cm2 significantly improves the surface hardness and modulus. However, the results on corrosion resistance reveal that zinc ion implantation degrades the corrosion behavior of Mg-Ca alloys. Thus, zinc is not a favorable element for the ion implantation treatment of biomedical Mg-Ca alloys.