In 2002 and 2005 the moss biomonitoring technique was applied to air pollution studies in the Republic of Macedonia in the framework of the International Cooperative Programme on Effects of Air Pollution on Natural Vegetation and Crops under the auspices of the United Nations Economic Commission for Europe (UNECE-ICP Vegetation) Convention on Long-Range Transboundary Air Pollution (LRTAP). In August 2005 samples of the terrestrial mosses Homolothecium lutescens and Hypnum cupressiforme were collected at 72 sites evenly distributed over the territory of the country, in accordance with the sampling strategy of the European moss survey programme. A total of 41 elements (Na, Mg, Al, Cl, K, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Br, Rb, Sr, Zr, Mo, Cd, Sb, I, Cs, Ba, La, Ce, Sm, Eu, Tb, Dy Hf, Ta, W, Hg, Pb, Th, and U) were determined by instrumental epithermal neutron activation analysis and atomic absorption spectrometry. Principal component analysis was used to identify and characterize different pollution sources. Distributional maps were prepared to point out the regions most affected by pollution and to relate this to known sources of contamination. A few areas, as in 2002, are experiencing particular environmental stress: Veles, Skopje, Tetovo, Radoviš and Kavadarci-Negotino, whereas the agricultural regions in the south, south-west, and south-east show median European values for most elements of mainly pollution origin. A significant increase in the content of Ni is noticed in the 2005 moss survey compared with 2002, due to the increased production of the ferro-nickel smelter in Kavadarci. A higher content of Cd, Hg, and Pb in 2005 relative to 2002 can be explained by pollution from the lead-zinc smelter in Veles, as well as the pollution that comes from the open slag waste dump of this smelter. Protection activities on the dump of slag from the former ferrochromium smelter located near Tetovo resulted in a lower content of Cr in the 2005 moss survey.