Abstract: To enhance the Young’s modulus (E) and strength of titanium alloys, we designed titanium matrix composites with interconnected microstructure based on the Hashin–Shtrikman theory. According to the results, the in-situ reaction yielded an interconnected microstructure composed of Ti₂C particles when the Ti₂C content reached 50vol%. With widths of 10 and 230 nm, the intraparticle Ti lamellae in the prepared composite exhibited a bimodal size distribution due to precipitation and the unreacted Ti phase within the grown Ti₂C particles. The composites with interconnected microstructure attained superior properties, including E of 174.3 GPa and ultimate flexural strength of 1014 GPa. Compared with that of pure Ti, the E of the composite was increased by 55% due to the high Ti₂C content and interconnected microstructure. The outstanding strength resulted from the strong interfacial bonding, load-bearing capacity of interconnected Ti₂C particles, and bimodal intraparticle Ti lamellae, which minimized the average crack driving force. Interrupted flexural tests revealed preferential crack initiation along the 001 cleavage plane and grain boundary of Ti₂C in the region with the highest tensile stress. In addition, the propagation can be efficiently inhibited by interparticle Ti grains, which prevented the brittle fracture of the composites.