Coal-bearing strata are widespread in the western Great Khingan Mountains. Abundant coal resources have been found in the Jurassic Alatanheli Groups, the Cretaceous Bayanhua Groups, the Damoguaihe Formation and the Yimin Formation. The organic geochemical characteristics were analyzed in combination with hydrocarbon source rock evaluation and molecular organic geochemistry experiments, and the coal gas potential of coal seams was evaluated. The source rock evaluation results indicated that the Mesozoic coal samples have the characteristics of high organic matter abundance (TOC>30%), low maturity (Ro values of approximately 0.6%), and type III composition. The hydrocarbon generation potentials of the Alatanheli Groups and Bayanhua Groups are high, while the generation potentials of the Damoguaihe Formation and the Yimin Formation are low. The results of geochemistry show that the depositional environment of the coal seam was a lacustrine, oxidizing environment with a low salinity, and the source of the organic matter was mainly higher plants. Affected by weak degradation, the coal seams mainly formed low-maturity gas of thermal catalytic origin. The Cretaceous coal seams contain a large amount of phytoplankton groups deposited in a low-stability environment affected by a transgression event, and the potential range varied widely. For the Jurassic coal seams, the depositional environment was more stable, and the coal seams feature a higher coal-forming gas potential.