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Recovery of iron from iron-rich diasporic bauxite ore via reductive roasting followed by magnetic separation has been explored recently. However, the efficiency of alumina extraction in the non-magnetic materials is absent. In this paper, a further study on the digestion of alumina by the Bayer process from non-magnetic material obtained after magnetic separation of reduced iron-rich diasporic bauxite with sodium salts was investigated. The results indicate that the addition of sodium salts can destroy the original occurrences of iron-, aluminum- and silicon-containing minerals of bauxite ore during reductive roasting. Meanwhile, the reactions of sodium salts with complex aluminum- and silicon-bearing phases generate diaoyudaoite and sodium aluminosilicate. The separation of iron via reductive roasting of bauxite ore with sodium salts followed by magnetic separation improves alumina digestion in the Bayer process. When the alumina-bearing material in bauxite ore is converted into non-magnetic material, the digestion temperature decreases significantly from 280 °C to 240 °C with a nearly 99% relative digestion ratio of alumina.