Hydroxyapatite (HAp) is the most widely used material for bio coating. The functional layer can be produced by many methods, however, the most perspective by its utility, easy to scale up, and simplicity aspects remains a hydrothermal treatment approach. In this work, an HAp coating was produced by low-temperature hydrothermal treatment on the ultrafine-grain beta Ti-xMo (x = 23, 27, 35 wt.%) alloys. The proposed surface treatment procedure combines acid etching, alkaline treatment (AT), and finally hydrothermal treatment (HT). The uniqueness of the approach relies on the recognition of the influence of the molar concentration of NaOH (5 M, 7 M, 10 M, 12 M) during the alkaline treatment on the growth of hydroxyapatite crystals. Obtained and modified specimens were examined structurally and microstructurally at every stage of the process. The results show that the layer after AT consist of titanium oxide and phases based on sodium with various phase relations dependent on NaOH concentration and base composition. The AT in 7 M and 10 M enables to obtain the HAp layer, which can be characterized as the most developed in terms of thickness and porosity. Finally, selected coated samples were investigated in terms of surface wettability test managed in time relation, which for the results confirm high hydrophilicity of the surfaces. Conducted research shows that the low-temperature hydrothermal processing could be considered for a possible adaptation in the drug encapsulation and delivery systems.