Nitriding and Carburizing methods are widely used to improve the performance of titanium alloy in terms of hardness and wear resistance. However, titanium alloy possesses low thickness of cementation layer and poor dyn mics. In this study, we propose a vacuum pulse carbonitriding (nitriding and carburizing) method which approaches to deposit a gradient reinforcement layer on the surface of TA2 titanium alloy. X-ray diffraction and scanning electron microscopy analyses were conducted to characterize the organizational structure and surface morphology of the new deposit layer. Results show that the order of the gas medium has different effects on the organizational structure and the performance of the carbonitriding layer. When the titanium alloy was treated with carburizing before nitriding, the cementation layer of TA2 formed a new compound phase mainly composed of TiN0.3, C0.7N0.3Ti, and TiN, with high hardness gradient. The effects of different processes on the properties of TA2 titanium alloy were also investigated. The corrosion rate of T(C,N) sample is lower than that of the raw sample four orders of magnitude. Moreover, the corrosion rate of the untreated sample are twice times the corrosion rate of the treated sample. Therefore, carbonitriding is the most promising strategy to strengthen the properties of TA2 titanium alloy.