Nanocrystalline diamond (NCD) film deposition on pure titanium and Ti alloys is extraordinarily difficult because of the high diffusion coefficient of carbon in Ti, the large mismatch in their thermal expansion coefficients, the complex nature of the interlayer formed during diamond deposition, and the difficulty to achieve very high nucleation density. In this investigation, NCD films were successfully deposited on pure Ti substrate by using a novel substrate pretreatment of ultrasonic scratching in a diamond powder-ethanol suspension and by a two-step process at moderate temperature. It was shown that by scratching with a 30-μm diamond suspension for 1 h, followed by a 10-h diamond deposition, a continuous NCD film was obtained with an average grain size of about 200 nm. Detailed experimental results on the preparation, characterization, and successful deposition of the NCD films on Ti were discussed.