In response to the complex issue regarding the influence of the liberation degree and particle size of pyrite in high-sulfur coal gangue on the sulfur recovery process through gravity separation, test and experimental methods such as the AMICS automatic quantitative analysis system, X-ray fluorescence spectrometer, and shaking table experiments, combined with the kinetic analysis of the shaking table separation process, were employed. The technological mineralogy characteristics of high-sulfur coal gangue and the influence of the liberation degree of pyrite in high-sulfur coal gangue on the migration law of gravity separation products were investigated. The results indicated that the ratio of pyrite to the total sulfur content in high sulfur coal gangue was as high as 87.16%, and pyrite was mostly associated with kaolinite in forms such as tabular, group aggregations, or lumps. When recovering pyrite from high-sulfur coal gangue using the shaking table, the lower limit of the effective separation particle size was 0.038 mm. The liberation of pyrite in the concentrate after separation was favorable, with a single liberation degree reaching as high as 82.37%. However, the pyrite in the re-election and roughing tailings had a more complex associated relationship with other minerals, and the single liberation degree of pyrite was relatively low. Meanwhile, the particle size and single liberation degree of coal gangue had a significant influence on their movement trajectories on the shaking table bed surface. When the single liberation degree of pyrite was lower than 85%, it would cause pyrite to be lost in the tailings to varying degrees.experiments, combined with the kinetic analysis of the shaking table separation process, were employed. The technological mineralogy characteristics of high-sulfur coal gangue and the influence of the dissociation degree of pyrite in high-sulfur coal gangue on the migration law of heavy separation products were investigated. The results indicated that the ratio of pyrite to the total sulfur content in high-sulfur coal gangue was as high as 87.16%, and pyrite was mostly associated with kaolinite in forms such as tabular, group aggregations, or lumps. When recovering pyrite from high-sulfur coal gangue using the shaking table, the lower limit of the effective separation particle size was 0.038 mm. The dissociation of pyrite in the concentrate after separation was favorable, with a single dissociation degree reaching as high as 82.37%. However, the pyrite in the re-election tailings and roughing tailings had a more complex associated relationship with other minerals, and the single dissociation degree of pyrite was relatively low. Meanwhile, the particle size and single dissociation degree of coal gangue had a significant influence on their movement trajectories on the shaking table bed surface. When the single dissociation degree of pyrite was lower than 85%, it would cause pyrite to be lost in the tailings to varying degrees.