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Pyrite has a significant effect on the spontaneous combustion of coal. The presence of pyrite can change the propensity of coal towards spontaneous combustion. The influences of various pyrite contents on the parameters of spontaneous combustion, such as index gases, temperature and released heat etc., were investigated in this study. Coal samples with different pyrite contents (0%, 3%, 5%, 7%and 9%) were made by mixing coal and pyrite. The oxidation experiments under temperature-programmed condition were carried out to test the release rate of gaseous oxidation products at different temperatures. Differential scanning calorimeter (DSC) was employed to measure the intensity of heat release during coal oxidation for various pyrite contents. The results indicate that pyrite can nonlinearly accelerate the process of spontaneous combustion. The coal sample with a pyrite content of 5% has the largest CO release rate and oxygen adsorption as well. However, the coal sample with a pyrite content of 7% has the largest rate of heat flow according to the results from the DSC tests. Pyrite contents of 5%–7% in coal has the most significant effects on spontaneous combustion within the range of this study. The conclusions are conducive to the evaluation and control for the spontaneous combustion of coal.