The microstructure and precipitate evolution of as-cast Mg–Nd alloys with different contents of Nd was investigated via experimental and simulation methods. The research showed that the as-cast microstructure of Mg–Nd alloy consisted of α-Mg dendrites and the intermetallic phases. A metastable β phase precipitated, followed by α-Mg dendrites that could be confirmed as Mg₁₂Nd by X-ray diffraction (XRD) analysis. The amount of β-Mg₁₂Nd presented a rising trend with increasing Nd additions. In addition, the tertiary phase was also observed in as-cast Mg–Nd alloy when Nd content was greater than 3 wt.%, which precipitated from the oversaturated α-Mg matrix. The tertiary phase should be β₁-Mg₃Nd, which is also a metastable phase with a face-centered cubic lattice. However, it is a pity that the tertiary phase was not detected by the XRD technique. Moreover, an effective cellular automaton (CA) model was explored and applied to simulate the time-dependent α-Mg/β₁-Mg₃Nd eutectic growth. The simulated results of α-Mg/β₁-Mg₃Nd eutectic growth in Mg-3Nd presented that the growth of α-Mg dendrites was accompanied by the nucleation and growth of β₁-Mg₃Nd precipitates and eventually formed a eutectic structure. The eutectic morphologies for Mg–Nd system alloys with different Nd contents were also simulated using the proposed model, and the results revealed that α-Mg dendrite was a refinement, and the amount of α-Mg/β₁-Mg₃Nd eutectic was promoted, with increasing Nd content.