The age-hardening responses and the corresponding microstructures of Mg-0.5Ca-xAl (x = 0, 0.1, 0.3, 0.5, 1 wt. %) alloys were investigated by hardness tests and transmission electron microscopy. For the optimum Al addition of 0.3 wt. % an enhanced age-hardening response with the highest peak hardness of HV=72 was achieved. TEM analyses confirmed that the improvement in the peak hardness is associated with the dense precipitation of ordered monolayer G.P. zones. Whereas, lower content of Al resulted in the formation of G.P. zones and Mg2Ca and the excess addition of Al causes the formation of the G.P. zones and the grain boundary Al2Ca phase.