The current research aim is to biofunctionalize pure titanium (Ti, grade IV) substrate with titania nanotubes and Zn doped hydroxyapatite-based coatings by applying a duplex electrochemical treatment, and to evaluate the influence of Zn content on the physico-chemical properties of hydroxyapatite (HAp). The obtained nanostructured surfaces were covered with HAp-based coatings doped with Zn in different concentrations by electrochemical deposition in pulsed galvanostatic mode. The obtained surfaces were characterized in terms of morphology, elemental and phasic composition, chemical bonds, roughness, and adhesion. The nanostructured surface consisted of titania nanotubes (NT), aligned, vertically oriented, and hollow, with an inner diameter of ~70 nm. X-ray Diffraction (XRD) analysis showed that the nanostructured surface consists of an anatase phase and some rutile peaks as a secondary phase. The morphology of all coatings consisted of ribbon like-crystals, and by increasing the Zn content the coating became denser due to the decrement of the crystals’ dimensions. The elemental and phase compositions evidenced that HAp was successfully doped with Zn through the pulsed galvanostatic method on the Ti nanostructured surfaces. Fourier Transform Infrared spectroscopy (FTIR) and XRD analysis confirmed the presence of HAp in all coatings, while the adhesion test showed that the addition of a high quantity leads to some delamination. Based on the obtained results, it can be said that the addition of Zn enhances the properties of HAp, and through proper experimental design, the concentration of Zn can be modulated to achieve coatings with tunable features.