Effects of industrial pollution on the behaviour of radionuclides in spruce forest ecosystems were studied along a gradient from of a copper-nickel smelter in Monchegorsk, NW Russia. A reference site was situated in Lapland, Finland, 152 km west of Monchegorsk. Most of the total 137Cs activity in soil was in mineral (E and B) horizons, except at the reference site where the major part was still in the organic surface layer. Most of the total 90Sr activity still remaining in the soil profile was found in the surface layer, but the relative amount decreased with increasing level of industrial pollution. Pollutants from the smelter clearly affected the chemical speciation of radionuclides. Smaller amounts of exchangeable radionuclides were present in the organic surface layer at the most polluted sites. The decline of 137Cs with decreasing distance from the smelter correlated strongly with a similar depletion in exchangeable K and Mg. Total concentrations of 137Cs and 90Sr showed high correlations with exchangeable cations, particularly in the E and upper B horizon. A sudden change in behaviour of 137Cs in the lower B horizon may be associated with changes in clay mineralogy along the soil profile caused by weathering.