Different bulk metallic glasses (BMGs) were prepared in ductile Cu47.5Zr47.5Al5, Zr62Cu15.4Ni12.6Al10, and brittle Zr55Ni5Al10Cu30 alloys by controlling solidification conditions. The achieved microstructures were characterized by x-ray diffraction, differential scanning calorimetry, transmission electron microscopy, and synchrotron- based high-energy x-ray diffraction. Monolithic BMGs obtained by high-temperature injection casting are brittle, while BMGs bearing some nanocrystals with the size of 3 to 7 nm and 2 to 4 nm, obtained by low-temperature injection casting and in situ suction casting, respectively, exhibit good plasticity. It indicates that the microstructures of BMGs are closely affected by the solidification conditions. Controlling the solidification conditions could improve the plasticity of BMGs.