Zr53.9Cu29.4Ni4.9Al9.8Fe2 alloy sample with the diameter of 3 mm was prepared by Cu mold suction casting at different temperatures. The effect of casting temperature on mechanical properties and microstructure of the as-cast alloy was investigated. It is found that there is a critical casting temperature for the fully amorphous structure, below which the crystallization phase might be precipitated. Experiment results show that the compressive strength increases and the compressive plasticity slightly decreases when the casting temperature increases to certain extent. However, the compressive strength and the compressive plasticity simultaneously increase when the casting voltage increases to 9 kV, and the compressive plasticity is 2.62%. Mechanical properties of BMG can be tailored to certain extent by controlling the casting temperature, which is correlated with free volume and residual stresses.