Abstract: A type of polymer/ceramic coating was introduced on a magnesium-based nanocomposite, and the nanocomposite was evaluated for implant applications. The microstructure, corrosion, and bioactivity of the coated and uncoated samples were assessed. Mechanical alloying followed by sintering was applied to fabricate the Mg–3Zn–0.5Ag–15NiTi nanocomposite substrate. Moreover, different contents of poly(lactic-co-glycolic acid) (PLGA) coatings were studied, and 10wt% of PLGA content was selected. The scanning electron microscopy (SEM) images of the bulk nanocomposite showed an acceptable homogenous dispersion of the NiTi nanoparticles (NPs) in the Mg-based matrix. In the in vitro bioactivity evaluation, following the immersion of the uncoated and coated samples in a simulated body fluid (SBF) solution, the Ca/P atomic ratio demonstrated that the apatite formation amount on the coated sample was greater than that on the uncoated nanocomposite. Furthermore, assessing the corrosion resistance indicated that the coatings on the Mg-based substrate led to a corrosion current density (i_corr) that was considerably lower than that of the substrate. Such a condition revealed that the coating would provide an obstacle for the corrosion. Based on this study, the PLGA/hardystonite (HT) composite-coated Mg–3Zn–0.5Ag–15NiTi nanocomposite may be suitably applied as an orthopedic implant biomaterial.