The in vitro and in vivo performance of hydroxyapatite (HAp) coatings can be modified by the addition of different trace ions, such as silicon (Si), lithium (Li), magnesium (Mg), zinc (Zn) or strontium (Sr) into the HAp lattice, to more closely mirror the complex chemistry of human bone. To date, most of the work in the literature has considered single ion-substituted materials and coatings, with limited reports on co-substituted calcium phosphate systems. The aim of this study was to investigate the potential of radio frequency magnetron sputtering to deposit Sr and Zn co-substituted HAp coatings using Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The FTIR and XPS results highlight that all of the Sr, Zn and Sr-Zn co-substituted surfaces produced are all dehydroxylated and are calcium deficient. All of the coatings contained HPO4 2− groups, however; only the pure HAp coating and the Sr substituted HAp coating contained additional CO32− groups. The XRD results highlight that none of the coatings produced in this study contain any other impurity CaP phases, showing peaks corresponding to that of ICDD file #01-072-1243 for HAp, albeit shifted to lower 2θ values due to the incorporation of Sr into the HAp lattice for Ca (in the Sr and Sr-Zn co-substituted surfaces only). Therefore, the results here clearly show that RF magnetron sputtering offers a simple means to deliver Sr and Zn co-substituted HAp coatings with enhanced surface properties.