We report on the formation of ultrafine-grained Ti66Nb13Cu8Ni6.8Al6.2 composites with in situ precipitated micrometer-sized β-Ti(Nb) phase by spark plasma sintering with crystallization. Microstructure analysis indicated that all alloys consisted of soft (Cu, Ni)Ti2 regions surrounded by hard β-Ti(Nb) regions but displayed different microstructures. The alloys exhibited high fracture strength of more than 2200 MPa and remarkable plasticity of ∼25%. The results provided a promising method for fabricating large-sized bulk composites with excellent mechanical properties by powder metallurgy.