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Chemical looping gasification (CLG) is an effective coal utilization technology. In this work, the CLG of bituminite was investigated through fixed-bed batch experiments using NiFe₂O₄ oxygen carrier (OC) to achieve high-quality syngas. The changes in the phase of the oxygen carrier during the chemical looping reaction and the reaction mechanism were explored. The results show that elevated temperature and adding a fraction of steam facilitate the gasification reaction. Adding an appropriate amount of ZrO₂ into the NiFe₂O₄ and modification with alkali metal can enhance the performance of the oxygen carrier. A carbon conversion of 95% and a syngas (CO and H₂) selectivity of 86% were obtained under the optimized reaction conditions of 950 °C, an oxygen-carrier-to-bituminite (O/B) ratio of 7:3, a NiFe₂O₄/ZrO₂ ratio of 7:3, and a steam rate of 0.08 mL/min. Modification of the NiFe₂O₄ by doping alkali metal can significantly facilitate the CLG process. Alkali lignin ash has a more pronounced modifying effect on oxygen carriers than K₂CO₃. The NiFe₂O₄ OC underwent a gradual reduction in Ni²⁺ → Ni and Fe³⁺ → Fe^8/3+ → Fe²⁺ → Fe processes during the gasification reaction phase. In addition, 20 redox cycles were conducted to demonstrate the oxygen carriers’ good cyclic reaction performance in the CLG process. After 20 redox cycles, the carbon conversion rate was maintained at about 90%, and the syngas selectivity was stably kept at over 80%. This work laid the theoretical foundation for the clean and efficient use of bituminite.