Microstructures and mechanical properties of Cu mold-cast Ti50Cu25Ni15Sn5Ta5 and Ti45Zr5Cu44Ni5Ta1 alloys were investigated by means of X-ray diffraction, electron microscopy and compressive testing. Ti50Cu25Ni15Sn5Ta5 alloys form microscopic composites consisting of Ti-based metallic glass as primary phase and β–Ti phases, while Ti45Zr5Cu44Ni5Ta1 alloys consisting of Ti-based metallic glass matrix and high density of nanocrystals dispersed in the matrix homogeneously. Ti50Cu25Ni15Sn5Ta5 bulk composite alloys showed 1.6% of plastic deformation and 2200 MPa of 0.2% of proof stress. The alloys also exhibited work hardening because of the presence of microscopic crystalline phases. Ti45Zr5Cu44Ni5Ta1 bulk alloys also deformed plastically after stress reached 2000 MPa without work hardening.