Titanium (Ti) has poor tribological and mechanical properties such as low hardness and wear resistance. In this study, we considerably improve Ti’s hardness by laser ablation method. Ambient air, N2 gas chamber and N2/liquid water environments were separately selected as irradiation environments and their effect was comparatively studied on Ti treatment surfaces. The fabrication of titanium nitride (TiN) structure was successfully confirmed by XRD analysis in N2 gas and N2/liquid water as irradiation media. Accordingly, there was good adhesion between TiN structure and Ti’s surface. Vickers hardness test indicated the laser treatment and TiN structure significantly improved Ti’s hardness.