In this study, ball-milled powder of Ti and Al was used to fabricate Ti–Al intermetallic compound-reinforced Al matrix composites by an in-situ reaction in cold-pressing sintering and hot-pressing sintering processes. The detailed microstructure of the Ti–Al intermetallic compound-reinforced Al composite was characterized by optical microscopy (OM), X-ray diffraction (XRD), energy dispersive spectrometry (EDS), and electron backscattered diffraction (EBSD). The results indicate that a typical core–shell-like structure forms in the reinforced particles. The shell is composed of a series of Ti–Al intermetallic compounds and has good bonding strength and compatibility with the Al matrix and Ti core. With cold-pressing sintering, the shell around the Ti core is closed, and the shell thickness increases as the milling time and holding time increase. With hot-pressing sintering, some radiating cracks emerge in the shell structure and provide paths for further diffusion of Ti and Al atoms. The Kirkendall effect, which is caused by the difference between the diffusion coefficients of Ti and Al, results in the formation of cavities and a reduction in density degree. When the quantity of the intermetallic compounds increases, the hardness of the composites increases and the plasticity decreases. Therefore, factors that affect the quantity of the reinforcements, such as the milling time and holding time, should be determined carefully to improve the comprehensive properties of the composites.