In the field of exploring the precursors of TiC/Ti composite, Cr2AlC was innovatively used as the precursor in this study. Based on the formation of TiC in pure Ti matrix during hot-pressing sintering, Al and Cr elements changed the microstructure of matrix to form TiC/(α + β)-Ti composite, and the reaction mechanism of Cr2AlC-Ti system in the sintering process was discussed in detail. During the cooling process, Cr element retained β-Ti to room temperature, and the uniformly distributed TiC was used as the nucleation site of α-Ti. By controlling the content of Cr2AlC added, the microstructure of the composite was regulated. In 10 vol% Cr2AlC/Ti composite, the α-Ti extend form the boundary of TiC to all sides, forming a microstructure of quasi-continuous network structure covering equiaxed β-Ti, which exhibited the optimal strength with ultimate tensile strength of 1184 MPa. The interface analysis shown that there is good interface bonding at TiC/α-Ti, which made the whole frame have good load transfer. And there were stacking faults at the TiC/β-Ti interface, meaning the obvious CTE mismatch strengthening at it.