This study investigated the effects of annealing environment for the densification and purification properties of pure titanium coating layer manufactured by cold spraying. The annealing was conducted at /1 h and three kinds of environments of vacuum, Ar gas, and mixture gas were controlled. Cold sprayed Ti coating layer (as sprayed) represented 6.7% of porosity and 228 HV of hardness, showing elongated particle shapes (severe plastic deformation) perpendicular to injection direction. Regardless of gas environments, all thermally heat treated coating layers consisted of pure -Ti and minimal oxide. Vacuum environment during heat treatment represented superior densification properties (3.8% porosity, 156.7 HV) to those of Ar gas (5.3%, 144.5 HV) and mixture gas (5.5%, 153.1 HV). From the results of phase analysis (XRD, EPMA, SEM, EDS), it was found that the vacuum environment during heat treatment could be effective for reducing oxide contents (purification) in the Ti coating layer. The characteristic of microstructural evolution with heat treatment was found to be different at three different gas environments. The controlling method for improving densification and purification in the cold sprayed Ti coating material was also discussed.