We report the enhanced precipitation-hardening response of Mg–0.5Ca (wt.%) alloy by microalloying with Al. The peak hardness of 50 HV for the binary alloy was enhanced to 72 HV in a ternary Mg–0.5Ca–0.3Al alloy. Transmission electron microscopy and 3D atom probe analyses confirmed that the improvement in the peak hardness is associated with the dense precipitation of ordered monolayer Guinier–Preston zones and the subsequent formation of Al2Ca causes the over-aging.