Magnesia refractory materials (MgO) exhibit outstanding refractory properties, with MgO-C products holding significant market prospects. In MgO-Al2O3-based refractory materials, ZrO2 was added, and the effect of ZrO2 addition on the performance of the refractory materials was studied. Using MgO and ZrO2 as raw materials, MgO and Al2O3 were incorporated into spinel in two different ways to prepare a novel MgO-MgO•Al2O3-ZrO2 castable. Research indicates that when the addition amounts of MgO and Al2O3 are 8%, the castable exhibits the best erosion resistance. Through comparison, it was found that the erosion resistance of Al2O3-Cr2O3 materials is inferior to that of the novel MgO-MgO•Al2O3-ZrO2 castable. Among them, high-alumina refractory materials within the aluminosilicate category have been widely applied in thermal power plants, coal plants, and cement kilns due to their adaptability and cost-effectiveness.