Formation of TiN by femtosecond laser processing in controlled gas atmosphere is reported. A dual-stage process was designed and aimed to first remove and restructure the native oxide layer of titanium surface through laser irradiation under an argon-controlled atmosphere, and then to maximize titanium nitride formation through an irradiation under a nitrogen reactive environment. An extensive XPS study was performed to identify and quantify laser-induced titanium surface chemistry modifications after a single-stage laser process (Ar and N2 individually), and a dual-stage laser process. The importance of each step that composes the dual-stage laser process was demonstrated and leads to the dual-stage laser process for the formation of TiO, Ti2O3 and TiN. In this study, the largest nitride formation occurs for the dual stage process with laser conditions at 4 W/1.3 J cm−2 under argon and 5 W/1.6 J cm−2 under nitrogen, yielding a total TiN composition of 8.9%. Characterization of both single-stage and dual-stage laser process-induced surface morphologies has been performed as well, leading to the observation of a wide range of hierarchical surface structures such as high-frequency ripples, grooves, protuberances and pillow-like patterns. Finally, water wettability was assessed by means of contact angle measurements on untreated titanium surface, and titanium surfaces resulting from either single-stage laser process or dual-stage laser process. Dual-stage laser process allows a transition of titanium surface, from phobic (93°) to philic (35°), making accessible both hydrophilic and chemically functionalized hierarchical surfaces.