Three types of ZrAlNiCu metallic glasses were successfully fabricated through vacuum arc melting under an argon atmosphere with suction-casting into a water-cooling-copper mold. The compressive mechanical properties of the three metallic glasses were tested using an Instron-3369 mechanical testing machine, and the compressive fracture surface was investigated by FEI Nano230 scanning electron microscope (SEM). Results show that increasing the Ni content and decreasing the Cu content will decrease the fracture strength and elastic modulus of the metallic glasses, and change the “vein-type” fracture surface to a completely brittle characteristic. The increase in the Ni content and decrease in the Cu content decrease the density of the free volume, degrade the deformation ability, increase the local deformation degree, and thus, decrease the fracture strength, plasticity and elastic modulus of the ZrAlNiCu metallic glass.