Titanium implant osseointegration can be enhanced by surface modifications that include hydroxyapatite from Ca3(PO4)2. However, CaO may provide more surface calcium (w/w) to induce cellular responses. Therefore, the purpose of this study was to compare responses to novel CaO and Ca3(PO4)2-enriched titania-polyester (PPC) nanocomposite coatings, which were created by an electrostatic ultrafine dry powder coating technique. EDX confirmed the presence of a base polymer scaffold, biocompatible titanium, and CaO or Ca3(PO4)2. SEM showed that human embryonic palatal mesenchymal cells (ATCC CRL-1486) had attached and spread out onto all surfaces within 24 hours. Cell attachment assays showed that there was a progressive increase in cell numbers with surface CaO incorporation (0–5%), such that the PPC + 5% CaO coatings supported the most cells. Furthermore, the PPC + 5% CaO had significantly more (P = 0.006) cells attached to their surfaces than the PPC + 5% CaP coatings and titanium controls, at 24 hours. The PPC + 5% CaO also had more cells that had proliferated on their surfaces over 72 hours, although these differences were not significant (P > 0.05). Similarly, MTT assays showed that the cells had sustained metabolic activity on all surfaces. Again, metabolic activities were highest on the PPC + 5% CaO, and they were significantly higher (P < 0.05) on all CaO-enriched surfaces (1/3/5% CaO) than on the PPC + 5% CaP. Subsequently, Alizarin Red-S staining detected the initiation of biomineralization within 2 weeks, and abundant mineral deposits after 4 weeks of growth on PPC + 5% CaO and PPC + 3% CaO. These nanocomposite coatings have shown that CaO enrichments may provide a heightened cell response when compared to conventional hydroxyapatite.