In order to systematically study the interface properties of Ti₂AlC/TiAl composite from an atomic perspective, based on the interface orientation relations obtained by the high resolution transmission electron microscope technique, the work of adhesion, interface energy and electronic structure of 24 Ti₂AlC/TiAl interface models with different terminations, different stacking sites, and different stacking sequences were calculated using the first principles calculation. The results show that the orientation relationship can be simplified to Ti₂AlC(0001)/TiAl(111); the surface energy of 7-layer TiAl(111) is 1.71 J/m², the surface energy at the Ti₂AlC(0001)-Al is the lowest (most stable) in the Al-rich and Ti-rich environments; among the 24 interface models, C-hcp-hollow-BCA has the largest work of adhesion (9.7180 J/m²) implying the strongest interface bonding strength, and Al-fcc-hollow-ACB has the smallest interface energy (0.3644 J/m²) meaning the strongest interface stability; while Ti(Al)-hcp-hollow-BAC is considered to be the most ideal interface structure, combining strong interface bonding strength and stability due to its high work of adhesion (3.9679 J/m²) and low interface energy (0.8630 J/m²), and the interface bonding at Ti(Al)-hcp-hollow-BAC is mainly from Ti-Ti metallic bonds and Ti-Al covalent bonds through the analysis of electronic structure.