Xinjiang Zhundong coal has abundant reserves and contains a relatively high content of alkaline earth metal elements. The high-calcium fly ash generated from its combustion serves as an excellent raw material for CO₂ sequestration. By adopting the atmospheric pressure direct wet carbonation process, research and optimization analysis were carried out on the carbonation of high-calcium fly ash, focusing on key parameters such as flue gas flow rate, temperature, and solid-liquid ratio. A kinetic model was constructed to determine the key factors and rate-controlling steps. Meanwhile, the performance of this process in chlorine removal and heavy metal removal was evaluated. It was found that, increasing the flue gas flow rate and reducing the solid-liquid ratio can effectively enhance the degree of carbonation per unit mass of fly ash. During the rapid carbonation stage (0~20 min), low temperature is beneficial for increasing the degree of carbonation, but the effect is not significant. In the rapid carbonation zone, the reaction of fly ash is mainly controlled by solid-film diffusion, with a correlation coefficient of 0.917 37 and an activation energy of 10.36 kJ/mol. After optimization by the response surface method, the optimal operating condition parameters are as follows: temperature of 57.1 ℃, flue gas flow rate of 2.86 L/min, and solid-liquid ratio of 200.0 g/L. Under these conditions, the average actual degree of carbonation reaches 30.2%. The chlorine content of the fly ash processed according to these parameters meets the requirements for reinforced products in the JC/T 409—2016 standard. For typical heavy metals such as arsenic and copper, the removal rates reach 88.4% and 55.6% respectively, indicating that this process has a certain detoxification ability. Therefore, the atmospheric wet carbonation of high calcium fly ash in Zhundong has great potential for application.