Body-centered cubic (BCC) Mg–Li alloy can be effectively strengthened by with the addition of Al and Zn. However, adding excessive amounts result in reduced mechanical properties and damping capacity of the alloy during subsequent heat treatment and deformation. The effects of solution-hot rolling-aging on the mechanical properties and damping capacity of LAZ1333 alloy and LAZ1366 alloy were studied. The solid solution strengthening greatly increases the hardness of the alloy, but the ductility is extremely poor. The AlLi softening phase precipitated during the subsequent hot rolling and aging process greatly improves the ductility of the alloy, but the excess precipitation of in the AlLi softening phase and the solid solution of excess Zn element are not conducive to the substantial improvement of the strength and ductility of the alloy. Excessive addition of alloying elements is detrimental to the damping capacity of the alloy, but the damping capacity of the alloy can be significantly improved by depleting the number of solute atoms through subsequent ageing treatments. The UTS and FE of as-cast LAZ 1333 alloy are 111 MPa and 16.9%, respectively. The as-aged LAZ1333 alloy has the best mechanical properties and damping capacity, and the UTS and FE are increased by 65.8% and 89.3%, respectively, compared to the as-cast alloy, and the damping capacity increased from 0.011 to 0.015.