In metal mining districts, element and radionuclide patterns in contaminated stream sediment can be used as tracers to detect and track the sources of pollution, and to distinguish geogenic from anthropogenic input, a prerequisite for rehabilitation planning. An example is given from the Mansfeld mining district in central Germany, where mining of ‘Kupferschiefer’ was conducted for over 800 years and led to extensive environmental pollution, considered to be mainly of geogenic origin. In consequence, only emergency measures have been implemented. The aim of the present study was to identify the metal sources in the mining district and to assess the range of pollutant migration. In combining conventional geochemistry, mineralogy and radiometry, it was shown that most of the multi-metal pollution in the Mansfeld mining district is of anthropogenic origin. The major sources of metals are low-grade ore, metalliferous flue dust and slag. Conventional geochemistry provided information on the spread of contamination in the rivers of the mining district. Mineralogy and microchemistry added data on the composition of the source material and pointed to the potential sources of contamination. Finally, the fraction of these sources in environmental pollution was estimated by gamma-spectroscopy.