Coal mining and coal combustion in thermal power plants (TPPs) are the major anthropogenic sources of arsenic (As) contamination in many different industrial regions. In this study of industrial regions of West Bengal and Singrauli, it is observed that there is an anthropogenic contribution to the contamination from As-bearing coal. Up to 14.53 mg/kg of As is obtained in coal of West Bengal which also has very high average Fe concentration (16,095 mg/kg) along with high concentration of Cu, Mn and Hg. Similar observations are also found in Singrauli Industrial Region where 3.14 mg/kg of As with very high concentration of Fe 43,867 mg/kg along with high Cu, Mn and Hg concentration is found in coal samples. This low-grade bituminous coal contains arsenopyrite as observed by SEM–EDX. Arsenopyrite is converted to arsenolite upon combustion in these TPPs as observed in XRD. The fly ash has average As concentration of 1.53 mg/kg for West Bengal and 2.38 mg/kg for Singrauli Industrial Region and high concentration of toxic elements. The soil near these TPPs and mining areas is enriched in As, Fe, Hg, Cu and Mn. Not only As but high concentrations of Fe, Hg, Mn are also observed from analysis of water which relates to the anthropogenic inputs. The dissolution of arsenolite in reducing environments caused by periodic flooding releases As into water. Hence, the As contamination in the study area also has anthropogenic origin from coal consumption in TPPs.