Effects of CaCO3 modificator on microstructure and mechanical properties of cast AZ91 Magnesium alloy have been investigated. Tensile fracture behavior of AZ91 alloys modified by CaCO3 has also been studied. Results show that CaCO3 modificator can obviously refine the grain of AZ91 magnesium alloy and Mg17Al12. Mg17Al12 in grain boundary of AZ91 alloy after modified by CaCO3 changes from continuous reticular structure to discontinuous reticular structure, even so much as granular structure and rod structure. After modified by 0.5wt% CaCO3 modificator, ultimate tensile strength, yield strength, impact toughness and elongation of AZ91 alloy increase from 186MPa to 200MPa, from 147MPa to 160MPa, from 4J to 9J and from 2.6% to 5%, respectively. And 0.5wt% CaCO3 modificator brings about an optimal refining effect. The study also shows that the fracture mechanism of modified AZ91 alloy is between cleavage fracture and quasi-cleavage fracture, which is as same as that of unmodified AZ91 alloy.