To overcome the tradeoff between strength and ductility of materials and obtain titanium matrix composites with excellent mechanical properties, in this study, the in situ-synthesized TiC particles and Ti-Al-V-Mo-Cr (Ti1400) alloy-reinforced Ti6Al4V (TC4) matrix composites ((Ti1400 + TiC)/TC4) were fabricated by low-energy ball milling and spark plasma sintering. The inhomogeneous distribution of TiC particles and Ti1400 alloy, as well as the compositional and structural transition zone, were characterized. The TiC/TC4 composite displayed a significantly higher yield strength and tensile strength compared to the TC4 alloy. However, the total elongation of the TiC/TC4 composite was only 57% of that in the TC4 alloy. In contrast, the (Ti1400 + TiC)/TC4 composites exhibited noticeably higher total elongation than the TiC/TC4 composite. Furthermore, the tensile strength of the composite increased with the increase in Ti1400 alloy content. The increase in strength can be attributed to solid solution strengthening and fine grain strengthening. The compositional and structural transition zone, formed by element diffusion, provided a better interface combination between the reinforcements and TC4 matrix. In the transition zone and Ti1400 region, a large number of α/β interfaces can effectively alleviate the stress concentration, and the increase in the β phase can bear more plastic deformation, which is conducive to improving the elongation of the composite. As a result, the (Ti1400 + TiC)/TC4 composites exhibited simultaneous improvements in strength and ductility.