The hydroxyapatite/Zinc Oxide (HA-TiO2/ZnO) coatings were grown on the Ti6Al4V substrate by plasma electrolyte oxidation from the CaP-based electrolyte containing 1, 3, and 6 g/L ZnO nanoparticles. XRD results confirmed the presence of ZnO, HA, and rutile phases in all coatings. According to SEM observations, coatings presented the porous morphology as a result of micro-arc discharges during the PEO process, whereas some of the pores in the composite coatings were filled by ZnO proportional to its content. After 7 days of immersion in SBF solution, accumulations of bone-like clusters were visible on the surface, demonstrating a promising bio-mineralization ability for all coatings, although the higher amount of 6 g/L ZnO had partially an inhibitory effect on the apatite nucleation. In-vitro studies demonstrated a time and concentration-dependent impact of ZnO on the viability of MG-63 osteoblast-like cells so that the concentration of 3 and 6 g/L caused the death of some cells after 7 days. The antibacterial tests also showcased that the presence of ZnO decreased the activity of gram-negative bacteria (E. coli) and gram-positive bacteria (S. aureus), while the higher concentration of ZnO particles led to more antibacterial activity of the coating. Finally, evaluating the corrosion behavior of PEO coatings through a potentiodynamic polarization test in Ringer's solution manifested a better protection against corrosion by increasing the ZnO content in the coating, mainly owing to the blocking of the pores by the ZnO particles, and as a result, the greater difficulty of electrolyte to reach the titanium substrate.