CaO-MgO-Al2O3-SiO2 glass-ceramics were successfully prepared using Baotou Steel BFS as the raw materials, choosing Fe2O3and Cr2O3 as nucleating agents. This paper focused on analyzing the combined effect of Fe2O3 and Cr2O3 on the structure andproperties of the glass-ceramics. Experimental results showed that the crystallization mechanism of glass-ceramics convertedsurface crystallization into bulk crystallization and the main crystalline phase of glass-ceramics changed gradually from augiteto diopside with the decrease of Fe2O3/Cr2O3 ratios. Therefore, an appropriate ratio of Fe2O3/Cr2O3 can act as nuclei forcrystallization of augite with integrated interlocking crystal structure and the physicochemical properties of glass-ceramic canbe improved. Consequently, the fracture mode of glass-ceramic was changed from intercrystalline to mixed transcrystalline/intercrystalline and therefore the average crack length can be shortened. Glass-ceramic with Fe2O3/Cr2O3 ratio of 1 had a highbending strength of 138.93 MPa, Vickers hardness of 7.51 GPa and acid resistance of 97.75%.