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In recent years, regenerative thermal oxidizer (RTO) has been widely used in the petroleum industry, chemical industry, etc. The massive storage required by solid waste has become a serious problem. Due to their chemical composition, bauxite tailings as raw materials for high-temperature thermal storage ceramics show enormous potential in the fields of research and application. In this study, we propose a method for preparing ferric-rich and high specific storage capacity by adding Fe2O3 powder to bauxite tailings. Based on a 7:3 mass ratio of bauxite tailings to lepidolite, Fe2O3 powder with different mass fractions (7 wt%, 15 wt%, 20 wt%, 30 wt%, and 40 wt%) was added to the ceramic material to improve the physical properties and thermal storage capacity of thermal storage ceramics. The results showed that ferric-rich thermal storage ceramics with optimal performance were obtained by holding them at a sintering temperature of 1000 °C for 2 h. When the Fe2O3 content was 15 wt%, the bulk density of the thermal storage ceramic reached 2.53 g/cm3, the compressive strength was 120.81 MPa, and the specific heat capacity was 1.06 J/(g·K). This study has practical guidance significance in the preparation of high thermal storage ceramics at low temperatures and low costs. [ABSTRACT FROM AUTHOR]