In 2000, the Barents Ecogeochemistry project detected very high concentrations of environmentally important and potentially harmful elements such as Tl and Cs in the topmost organic soil layer to the north and east of the Gulf of Finland. In 2003, additional organic soil layer (humus) and terrestrial moss samples were collected from the Baltic countries. These samples, together with selected samples from the Barents Ecogeochemistry project, were used to define the distribution of elements in terrestrial mosses and the organic soil layer in the eastern Baltic region. Cs isotopes from the fallout following the Chernobyl nuclear power plant accident in 1986 were still clearly detectable in the organic soil layer. The source of Tl detected in SE Finland and along the northern coast of Estonia is mainly emissions from the cement industry and power plants that use oil shale as fuel, but also geogenic dust from feldspar-rich minerogenic soil. Heavy metals and other elements detected in organic soil were estimated to be mostly geogenic in origin, but include fingerprints of older emissions from local industries. In mosses, their origin is either recent anthropogenic emission or, in many cases, local geogenic dust from open areas. Besides Cs isotopes from Chernobyl, no other long range airborne transportation of heavy metals, e.g. from the industrial areas of Central Europe, was detected.