This paper reports methods and results of the investigation of natural radionuclides levels in multiple media in the bone-coal mine areas in Hubei, Hunan, Jiangxi, Zhejiang, and Anhui Provinces. In the studied bone-coal mine areas, the specific activities of ²³⁸U and ²²⁶Ra in the soil samples were 0.37 and 0.24 Bq/g, respectively; the specific activities of ²²⁶Ra in the samples of bone-coal, bone-coal cinder and bone-coal cinder brick (BCCB) were 1.3, 1.4 and 0.9 Bq/g, respectively. In the water samples collected from the bone-coal mine areas, the average concentrations of natural uranium and ²²⁶Ra were 33µg/L and 58 mBq/L, respectively, while in the water samples collected from outside the bone-coal mine areas, they were 3.4µg/L and 45 mBq/L, respectively. In addition, the specific activities of ²³⁸U and ²²⁶Ra in air aerosol samples from the bone-coal mine areas were 0.6 and 0.5 mBq/m³, respectively.