Data comprise estimates of activity concentrations of naturally occurring radionuclides (40K, 238U and 232Th series radionuclides) in environmental media (soil and stream sediments and waters) and non-human biota (focusing on the ICRP Reference Animals and Plants). For soil, stream sediments and stream waters data were derived from total K, U and Th concentrations mainly from the ongoing geochemical survey of the United Kingdom (G-BASE), conducted by the British Geological Survey. The geochemical survey data are currently incomplete for England and Wales, but almost complete coverage was obtained for K in stream sediments by using the Wolfson Atlas data for southern England. For U and Th in sediments and K, U and Th in soils, more complete coverage was achieved by geological extrapolation (using relationships between soils/sediments and bedrock/superficial geology). For media and sediments, datasets are provided for both: (i) geometric mean concentrations from measured samples on a 5 x 5 km square basis where data are available; and (ii) extrapolated surfaces covering all of England and Wales. Data for non-human biota are from targeted sampling and analyses and data review.