In order to improve the mechanical properties of Mg-Li alloy with single β phase structure, Mg-12Li-3Al-xNd (x=0.3, 0.7, 1.1, 2.0wt.%) alloy was prepared. Subsequently, the as-cast microstructure and mechanical properties were observed and tested. The results showed that the structure of Mg-12Li-3Al-xNd (x=0.3, 0.7, 1.1, 2.0wt.%) as-cast alloy was composed of β phase matrix and Al2Nd, Al11Nd3, MgLiAl2, Al4Li9 and AlLi phases. With the increase of Nd content in the alloy, the Al-Nd intermetallic compounds have a trend to change from needle-like Al11Nd3 to granular Al2Nd. The hardness of as-cast Mg-12Li-3Al-xNd (x=0.3, 0.7, 1.1, 2.0wt.%) alloy was stable at room temperature. The tensile strength of Mg-12Li-3Al-1.1Nd was as high as 180 MPa, the elongation rate of Mg- 12Li-3Al-0.7Nd reached 53.7%, and the comprehensive mechanical properties of Mg-12Li-3Al-2.0Nd was the best. PLC phenomenon occurred during the tensile process of the alloys at room temperature. Therefore, the β-based Mg-Li alloy with good plasticity as well as enhanced strength can be obtained by a moderate addition of Nd and Al.