Photocatalysis-enhanced surface deposition on titanium surfaces for biomedical applications is investigated in this work. Immersion tests of commercially pure titanium (CP-Ti) pieces in a simulated body fluid adding bovine serum albumin (BSA) under ultraviolet (UV) irradiation in situ are carried out. The morphologies of deposition are characterized by SEM and stereo imaging microscopy, and the quantity and composition of the deposition is examined by SEM, energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy. The results show a deposition layer with thickness 89 μm is produced on 600 °C heat-treated specimens. An irradiation pattern of lighting/dark repeated results in more deposition on heat-treated CP-Ti. It is confirmed that a mixture of anatase and rutile phases generated on 600 °C heat-treated specimens has enhanced photocatalysis. The decomposition of BSA by photocatalysis, a possible product of nitrite also results in enhanced deposition on Ti. EDS analysis shows large reduction of carbon in the deposition on UV-light exposed surfaces compared to no UV-light-exposed surfaces. Furthermore, C–H bond decreases and C–C, Ca–O, and P–O bond increases are found on photoactivated surfaces. The deposition produced by this method is expected to be useful for applications to biomaterials with high bioactivity.