Nano-sized HA (nHA) was applied to the surface of glass and titanium substrates using electrostatic atomisation spray (EAS) deposition. The phase purity of nHA was confirmed by X-ray diffraction. The nHA suspension consisted of rod–like particles 20-30nm in width and 50-100nm in length. The viscosity and conductivity of nHA suspension were 321 mPa s and 5.6 x 10-4 S/m, respectively. EAS of nHA in cone-jet mode was achieved at flow rate of 10-9 m3s-1 with the applied voltage between the needle and the ring-shaped ground electrode of ~6 kV. Micrometer- to submicrometerscaled nHA islands were successfully deposited on the substrate surface. Image analysis showed that the area percentage of nHA increased with deposition time, it covered 50% of the surface area after 10s of spraying. Partial dissolution of nHA was observed after immersion in deionised water for 1 month, particularly on the submicrometer sized nHA islands. Formation of a bone-like apatite layer was found after incubation in simulated body fluid (SBF K9) for 5 days, indicating the high bioactivity of the nHA deposits. In vitro culture with human osteoblast cells showed that the nHA islands were able to support the growth of HOB cells during 7 days of culture; the HOB cell activity increased with culture time as well as EAS deposition time. Immunofluorescence study showed that HOB cells expressed well-organised actin stress fibres on nHA deposited surfaces after 3 days of culture. The result indicated that nHA deposition provided more favourable surfaces for cell attachment. Therefore, electrostatic atomization spray deposition of nHA offers great potential for the creation of bioactive surfaces on bioinert implant surface to provide improved interfacial bonding with host tissues.