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In-situ electron irradiation and aging are applied to introduce high-density precipitates in an Mg-10Gd-3Y-1Zn-0.5Zr (GWZ1031K, wt.%) alloy to improve the hardness. The results show that the hardness of the Mg alloy after irradiation for 10 h and aging for 9 h at 250 °C is 1.64 GPa, which is approximately 64% higher than that of the samples before being treated. It is mainly attributed to γ′ precipitates on the basal plane after irradiation and the high-density nanoscale β′ precipitates on the prismatic plane after aging, which should be closely related to the irradiation-induced homogenous clusters. The latter plays a key role in precipitation hardening. This result paves a way to improve the mechanical properties of metallic materials by tailoring the precipitation through irradiation and aging.