In this work, intermetallic materials based on γ-TiAl in situ strengthened with the Ti3Al phase have been obtained from the initial components of titanium and aluminum under the conditions of free SHS-compression in one technological step and in ten seconds. This method combines the process of the combustion of initial components in the mode of self-propagating high-temperature synthesis (SHS) with high-temperature shear deformation of the synthesized materials. The following initial compositions have been studied (mol): Ti–Al, 1.5 Ti–Al, and 3 Ti–Al. Thermodynamic calculations have been carried out and the actual combustion temperature of the compositions under study has been measured. To increase the exothermicity of the studied compositions, a “chemical furnace” based on a mixture of Ti–C powders has been used, which allows us to increase the combustion temperature and stabilize the combustion front. It has been found that the actual combustion temperature of the selected compositions increased from 890–1120 to 1000–1350 °C. The results of X-ray powder diffraction and SEM are presented, mechanical and tribological characteristics of the obtained materials are measured, and 3D images of wear grooves are given. It has been found that a decrease in Ti molar fraction and an increase in Al molar fraction in the initial mixture lead to an increase in the mechanical (hardness up to 10.2 GPa, modulus of elasticity up to 215 GPa) and tribological characteristics (wear up to 4.5 times, coefficient of friction up to 2.4 times) of intermetallic materials.