Electrolytic manganese slag materials can be used in the preparation of glass‐ceramics. Herein, glass‐ceramics with excellent properties are obtained by melting electrolytic manganese slag and ferrochrome slag as raw materials. The effects of the addition of ferrochrome slag on the recrystallization of the base glass and the physicochemical properties of the glass‐ceramic are especially investigated. With the addition of ferrochrome slag, the introduced Cr2O3 may play a role in the deconstruction of the glass network and is more likely to produce a spinel phase as a way to promote the heterogeneous nucleation of the diopside phase. The sample with a ferrochrome slag addition of 12 wt% shows the optimal recrystallization ability. Furthermore, the ratio of nonbridging oxygen atoms (NBO) to the total amount of oxygen atoms (T) is the highest (NBO/T = 1.90). Also, the bending strength and the density of the samples reach 96.08 MPa and 3.05 g cm−3, respectively, and the acid and alkali resistance become 98.16% and 99.48%, respectively. Moreover, the glass‐ceramic structure did effectively stabilize and solidify the harmful heavy metal elements. This study has provided innovative ideas for an efficient, harmless, and low‐cost treatment of electrolytic manganese slag in the preparation of glass‐ceramics.