Moss biomonitoring technique was used for a heavy-metal pollution study in Macedonia in the framework of the International Cooperative Program on Effects of Air Pollution on Natural Vegetation and Crops (UNECE IPC Vegetation). Moss samples (n = 72) were collected during the summers of 2002, 2005, and 2010. The contents of 41 elements were determined by neutron activation analysis, atomic absorption spectrometry, and inductively coupled plasma atomic emission spectrometry. Using factor and cluster analyses, three geogenic factors were determined (Factor 1, including Al, As, Co, Cs, Fe, Hf, Na, Rb, Sc, Ta, Th, Ti, U, V, Zr, and rare-earth elements–RE; Factor 4 with Ba, K, and Sr; and Factor 5 with Br and I), one anthropogenic factor (Factor 2, including Cd, Pb, Sb, and Zn), and one geogenic-anthropogenic factor (Factor 3, including Cr and Ni). The highest anthropogenic impact of heavy metal to the air pollution in the country was from the ferronickel smelter near Kavadraci (Ni and Cr), the lead and zinc mines in the vicinity of Makedonska Kamenica, Probištip, and Kriva Palanka in the eastern part of the country (Cd, Pb, and Zn), and the former lead and zinc smelter plant in Veles. Beside the anthropogenic influences, the lithology and the composition of the soil also play an important role in the distribution of the elements.