To extend the materials application and achieve composite structures with combined advantages, the Cf/Al composites were joined with TiAl intermetallics by a novel laser-induced self-propagating high-temperature synthesis joining method. In this study, a Ni-Al-Zr interlayer was designed based on the calculation of the adiabatic temperature. The joint microstructure was characterized using scanning electron microscopy (SEM), energy dispersive spectrometry (EDS), transmission electron microscope (TEM) and X-ray diffraction (XRD). The results showed that the NiAl+Ni2AlZr+Ni3Al5Zr2 eutectic were produced during the joining. The Al3NiTi2, Ni2Al3 and NiAl3 reaction layers formed respectively on both sides. A nanoscale thin Zr-C reaction layer formed on the NiAl3/Cf interface and greatly enhanced the bonding quality on the Cf/Al side. The effect of the interlayer composition and joining pressure on the joint microstructure and mechanical property was investigated. The highest joint shear strength was 68.71MPa at a pressure of 4MPa when the Zr content was 5wt.%.