The magnesium-lithium (Mg-Li) alloy exhibits two phase structures between 5.7wt% and 10.3wt% Li contents, consisting of the a (hcp) Mg-rich and the β (bcc) Li-rich phases, at room temperature. In the experiment, Mg-5Li-2Zn, Mg-9Li-2Zn, Mg-16Li-2Zn, Mg-22Li-2Zn, Mg-5Li-2Zn-2Ca, Mg-9Li-2Zn-2Ca, Mg-16Li-2Zn-2Ca, and Mg-22Li-2Zn-2Ca (wt%) were melted. During the melting process, the flux, which was composed of lithium chloride (LiCl) and lithium fluoride (LiF) in the proportion of 3:1 (mass ratio) and argon gas were used to protect the alloys from oxidation. The microstructure, mechanical properties, and cold-rolling workability of the wrought alloys were studied. The crystal grain of the alloys (adding Ga) is fine. The hardness of the studied alloys decreases with an increase in element Li. The density of the studied alloys is in the range of 1.187 to 1.617 g/cm³. The reduction of the Mg-16Li-2Zn and Mg-22Li-2Zn alloys can exceed 85% at room temperature. The Mg-9Li-2Zn-2Ca alloy was heat treated at 300℃ for 8, 12, 16, and 24 h, respectively. The optimum heat treatment of the Mg-9Li-2Zn-2Ca alloy is 300℃×12h by metallographic observation and by studying the mechanical properties of the alloys.