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In this research, the coarse manganese concentrate was collected from a manganese ore concentrator in Tongren of China, and the contents of manganese and iron in coarse manganese concentrate were 28.63% and 18.65%, respectively. The majority of the minerals in coarse manganese concentrate occur in rhodochrosite, limonite, quartz, olivine, etc. Calcium chloride, calcium hypochlorite, coke, and coarse manganese concentrate were placed in a roasting furnace to conduct segregation roasting, which resulted in a partial chlorination reaction of iron to produce FeCl₃, ferric chloride reduced to metallic iron and adsorbed onto the coke, and rhodochrosite broken down into manganese oxide. Iron was extracted from the roasted ore using low-intensity magnetic separation, and manganese was further extracted from the low-intensity magnetic separation tailings by high-intensity magnetic separation. The test results showed that iron concentrate with an iron grade of 78.63% and iron recovery of 83.60%, and manganese concentrate with a manganese grade of 54.04% and manganese recovery of 94.82% were obtained under the following optimal conditions: roasting temperature of 1273 K, roasting time of 60 min, calcium chloride dosage of 10%, calcium hypochlorite dosage of 5%, coke dosage of 10%, coke size of −1 mm, grinding fineness of −0.06 mm occupying 90%, low-intensity magnetic field intensity of 0.14 T, and high-intensity magnetic field intensity of 0.65 T. Most minerals in the iron concentrate were Fe, Fe₃O₄, and a small amount of SiO₂ and CaSiO₃; the main minerals in the manganese were MnO, and a small amount of Fe₃O₄, SiO₂, and CaSiO₃. The thermodynamic calculation results are in good agreement with the test results.