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Non-isothermal oxidation is one of the important issues for the safe application of Ti-Al alloys, so this study aimed to illustrate the non-isothermal oxidation behaviors and the corresponding mechanisms of a TiAl-based alloy in comparison with a Ti₃Al-based alloy. The non-isothermal oxidation behaviors of Ti-46Al-2Cr-5Nb and Ti-24Al-15Nb-1.5Mo alloys in pure oxygen were comparatively investigated with a thermogravimetry-differential scanning calorimetry (TGA/DSC) simultaneous thermal analyzer heating from room temperature to 1450 °C with a heating rate of 40 °C/min. When the temperature rose above 1280 °C, the oxidation rate of the Ti-46Al-2Cr-5Nb alloy sharply increased and exceeded that of the Ti-24Al-15Nb-1.5Mo alloy owing to the occurrence of internal oxidation. When the temperature was higher than 1350 °C, the oxidation rate of the Ti-46Al-2Cr-5Nb alloy decreased obviously due to the generation of an oxygen-barrier β-Al₂TiO₅-rich layer by a chemical reaction between Al₂O₃ and TiO₂ in the oxide scale. Based on Wagner’s theory of internal oxidation, the reason for the occurrence of internal oxidation in the Ti-46Al-2Cr-5Nb alloy is the formation of the α phase in the subsurface, while no internal oxidation occurred in the Ti-24Al-15Nb-1.5Mo alloy due to the existence of the β phase in the subsurface with the enrichment of Nb and Mo.