In this work, Ti-5111 alloys with equiaxed, bimodal and lamellar microstructures were prepared by various heat treatment processes. The room-temperature tensile properties, deformation microstructure and fracture mechanism of the alloys with different microstructures were investigated. Furthermore, the mechanism by which the microstructure affects the mechanical properties of Ti-5111 alloys with three typical microstructures was confirmed. The Ti-5111 alloy with a bimodal microstructure has minimum grain size and a large number of αs/β phase boundaries, which are the primary reasons for its higher strength. Simultaneously, the excellent coordination in the deformation ability between the lamellar αs and β phases is what enables the alloy with a bimodal microstructure to have the most outstanding mechanical properties. Additionally, the presence of a grain boundary α phase and the parallel arrangement of a coarse αs phase are the main reasons for the inferior mechanical properties of the Ti-5111 alloy with a lamellar microstructure. The fracture mechanism of the alloy with an equiaxed microstructure is a mixed fracture mechanism including ductile fracture and destructive fracture. The fracture mechanisms of the Ti-5111 alloy with bimodal and lamellar microstructures are typical ductile fracture and cleavage fracture, respectively. These findings serve as a guide for the performance improvement and application of the Ti-5111 alloy.