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Phase relationships of the Mg–Nd–Zn system at the Mg-rich region are investigated through evaluation of selected compositions in the heat-treated conditions. Thermodynamic reassessment of the Mg–Nd–Zn system at the Mg-rich region is then carried out on the basis of both our experimental data and literature results. The calculated isothermal and vertical sections using current thermodynamic description are in good agreement with the experimental data. The metastable Mg 12 Nd phase was introduced into current thermodynamic description due to its metastability under solidification conditions. The solidification paths are simulated using computational thermodynamics coupled with the Scheil model by suppression of the Mg 41 Nd 5 phase and reasonable agreement is found with the microstructure evolution of as-cast Mg–Nd–Zn alloys.