The effects of Zn addition on the microstructure and tensile properties of as-extruded Mg-2Al-0.5Ca-xZn (x = 0, 0.3, 0.6, 0.9 wt.%) alloys were investigated in this work. The results showed that the extruded sheets exhibited a completely dynamically recrystallized microstructure, the grain size was refined, and texture weakening was achieved with Zn addition because of the segregation of Zn atoms on grain boundaries, which suppresses the growth of dynamic recrystallized grains. The addition of 0.6 wt.% Zn improved both the tensile strength and ductility of the as-extruded Mg-2Al-0.5Ca alloy. The as-extruded Mg-2Al-0.5Ca-0.6Zn alloy showed a 0.2% proof stress of 145 MPa, an ultimate tensile strength of 317 MPa, and an elongation of 30.0% along the extruded direction. The simultaneous improvement of strength and ductility was mainly due to the fine and homogeneous grain microstructure and the weakened extrude direction (ED)-tilted texture. The as-extruded Mg-2Al-0.5Ca-0.6Zn alloy showed little in-plane anisotropic tensile properties, with a 0.2% proof stress, ultimate tensile strength, and elongation in the 45° direction of 148 MPa, 299 MPa, and 25.0%, and those in the transverse direction of 148 MPa, 269 MPa, and 16.8%, respectively.