In order to solve the technical bottleneck of automatic detection technology of coal and gangue in the fully mechanized top coal caving mining, the low radiation level radioactivity measurement method is adopted to detect coal gangue mixed degree in coal releasing process, based on the radiation differentiation characteristics of natural γ-rays from coal and gangue. The research team analyzed the distribution characteristics of natural γ-rays in coal and rock layers of thick coal seams and the applicability of this method, introduced the basic principle of coal-gangue detection technology based on natural γ-ray, developed forming the test system about automatic coal-gangue detection, studied the radiation characteristics of coal and gangue, proposed determination model of the coal-gangue mixed degree, combined with the time sequence characteristics of the top coal’s releasing flow and the energy spectrum characteristics of different layers of rock, realized the precise coal-gangue detection technology in complex structure thick coal seam with multiple gangue. Field tests were conducted in Lilou, Xiaoyu and Tashan Coal Mine. The test results were well corroborated with the research results and achieved the expected results, which laid the foundation for the field application of intelligent coal mining.