The high-velocity suspension flame spraying technique (HVSFS) was employed in order to deposit 45S5 bioactive glass coatings onto titanium substrates, using a suspension of micron-sized glass powders dispersed in a water + isopropanol mixture as feedstock. By modifying the process parameters, five coatings with different thickness and porosity were obtained. The coatings were entirely glassy but exhibited a through-thickness microstructural gradient, as the deposition mechanisms of the glass droplets changed at every torch cycle because of the increase in the system temperature during spraying. After soaking in simulated body fluid, all of the coatings were soon covered by a layer of hydroxyapatite; furthermore, the coatings exhibited no cytotoxicity and human osteosarcoma cells could adhere and proliferate well onto their surfaces. HVSFS-deposited 45S5 bioglass coatings are therefore highly bioactive and have potentials as replacement of conventional hydroxyapatite in order to favour osseointegration of dental and prosthetic implants.