Calcium phosphate materials, particularly hydroxyapatite (HA), are extensively used in biomedical applications because of their prominence as primary inorganic constituents of human hard tissues. This study investigates the synthesis of HA coatings via spray pyrolysis using various precursors, including HA derived from bovine bone. The effects of pH on the formation and properties of HA coatings were systematically examined. Samples exposed to acidic conditions or left without pH adjustment led to the formation of HA, contrasting with the outcomes observed through dissolution methods. Different characterization techniques, such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray diffraction (XRD), were employed to evaluate the quality and crystallinity of the coatings. Among the samples, those exhibiting superior crystallinity and nanostructured features, including bovine HA, were selected for further surface functionalization with the antibiotic enrofloxacin using spin coating. As expected, the antibiotic loading on each material's surface depended on the amount of HA deposited on the substrate. However, the desorption results indicated that, in all cases, desorption persisted beyond 38 h, implying that HA-loaded matrices could be effective systems for controlled and prolonged drug release, which could be useful in dental or orthopedic implants for inhibiting the growth of bacterial biofilms.