The effect of solution treatment time on the microstructure and mechanical properties of aged the Mg-2.0Nd-2.0Sm-0.4Zn-0.4Zr (wt.%) alloy were investigated to give full play to the performance of the alloy. As the solution treatment time increased from 2 h to 12 h at 788 K, the grain size of the solution-treated alloy significantly increased, and the network-like β-Mg₁₂(Nd, Sm, Zn) phase gradually dissolved into the α-Mg matrix. It should be noted that no obvious residual β phase can be observed when the solution treatment time was more than 8 h. After the solution-treated alloy was further aged at 473 K for 18 h, a large number of nanoscale precipitates were observed in the α-Mg matrix. The solution treatment time was 2 h, the α-Mg matrix mainly consisted of spherical-shaped and basal plate-shaped precipitates. Upon the increase of solution treatment time to 8 h, the key strengthening phases transformed from spherical-shaped precipitates and basal plate-shaped precipitates to prismatic plate-shaped β′ precipitates. The orientation relationship between β′ precipitates and α-Mg matrix was ($\overline{1}$10)_β′ // (1$\overline{1}$00)_α and [112]_β′ // the [22$\overline{4}$3]_α. Further increasing of solution treatment time from 8 h to 12 h, the key strengthening phases mainly were still β′ precipitates. The solution treatment of aged alloy was carried out at 788 K for 8 h, which achieved optimal ultimate tensile strength (UTS) of 261 ± 4.1 MPa, yield strength (YS) of 154 ± 1.5 MPa, and elongation of 5.8 ± 0.1%, respectively.