TiAl intermetallic alloy at 1060 °C for 10 min. The interfacial microstructures and mechanical properties were investigated, and the enhancing mechanism of the joint strength was elucidated. The results showed that a perfect interface joint was achieved by using TiNiSi to braze the C/C composite. Ductile Ti 3 SiC 2 carbide was formed at the interface, which is beneficial to the joint bonding effect. The direct joining between the C/C composite and TiAl alloy using TiNiSi filler metal was unsuccessful, which was attributed to the high content of intermetallic compounds and hard-brittle phases in the brazed joint. The addition of a Cu interlayer to the joint can adjust the interfacial structure and reduce the content of brittle compounds, leading to a complete connection between the C/C composite and TiAl alloy. The interfacial transition layer on the C/C composite side mainly consisted of Ti 3 SiC 2 , Ti 3 AlC ductile ceramic phases, and TiC phase, which enhanced the performance of the brazed joint. The average shear strength at room temperature was 18.8 MPa, with the maximum value of 23.6 MPa, and the average shear strength at 600 °C was 25.8 MPa.