The distribution and enrichment of naturally occurring radioactive materials (NORM) in coal combustion residuals (CCRs) from different coal source basins have not been fully characterized in the United States. Here we provide a systematic analysis of the occurrence of NORM ((232)Th, (228)Ra, (238)U, (226)Ra, and (210)Pb) in coals and associated CCRs from the Illinois, Appalachian, and Powder River Basins. Illinois CCRs had the highest total Ra ((228)Ra + (226)Ra = 297 ± 46 Bq/kg) and the lowest (228)Ra/(226)Ra activity ratio (0.31 ± 0.09), followed by Appalachian CCRs (283 ± 34 Bq/kg; 0.67 ± 0.09), and Powder River CCRs (213 ± 21 Bq/kg; 0.79 ± 0.10). Total Ra and (228)Ra/(226)Ra variations in CCRs correspond to the U and Th concentrations and ash contents of their feed coals, and we show that these relationships can be used to predict total NORM concentrations in CCRs. We observed differential NORM volatility during combustion that results in (210)Pb enrichment and (210)Pb/(226)Ra ratios greater than 1 in most fly-ash samples. Overall, total NORM activities in CCRs are 7-10- and 3-5-fold higher than NORM activities in parent coals and average U.S. soil, respectively. This study lays the groundwork for future research related to the environmental and human health implications of CCR disposal and accidental release to the environment in the context of this elevated radioactivity.