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High-iron Bayer red mud, containing over 30% of iron, is considered low-grade iron ore. Due to the global iron deficiency in recent decades, the effective utilization of the iron contained in high-iron red mud has received increasing attention. In this work, a technological scheme was developed for the extraction of iron into cast iron from red mud by smelting reduction, followed by rapid cooling to separate the metal from the slag. The influence of various experimental parameters, including temperature, basicity, and reduction time, on the recovery of iron from red mud was studied in detail. The results demonstrated that the separation of metal from slag was complete. The maximum extraction of iron into cast iron was obtained at a temperature of 1450 °C, with approximately 88.5% achieved in the absence of sodium carbonate and 91.5% with sodium carbonate. The optimal experimental result is of great importance for the large-scale and highly efficient recycling of red mud. [ABSTRACT FROM AUTHOR]