Commercial purity titanium (CP-Ti) and a Ti-6Al-4V alloy (Ti64) were processed by high-pressure torsion (HPT) for 10 and 20 turns. The HPT processing produced a nanostructured microstructure and a significant strength enhancement in the CP-Ti and Ti64 samples. After 20 turns, the samples of HPT-processed CP-Ti and Ti64 were subjected to laser surface treatments in an air atmosphere using different scanning speeds and laser powers. The surface roughness of the laser-modified samples increased with increasing laser power and this produced hydrophilicity due to a lower contact angle. After a holding time of 27 days, these samples underwent a hydrophilic-to-hydrophobic transformation as the contact angle increased from 13° to as much as 120° for the CP-Ti sample, and for the Ti64 sample the contact angle increased from 10° to 126°. In addition, the laser surface modification process was carried out with different atmospheres (air, vacuum and O2) on heat-treated but unstrained CP-Ti and Ti64 samples and the contact angle changed due to the surface element content. Thus, as the carbon content increased from 28% to 47% in CP-Ti in a vacuum environment, the surface contact angle increased from 22° to 140°. When a laser surface modification process is conducted under oxygen-less conditions, it is concluded that the contact angle increases rapidly in order to control the hydrophobic properties of Ti and the Ti alloy.