Monitoring hazardous air pollutants is needed for understanding their spatial and temporal distribution and ultimately to minimize their harmful effects. For the first time, the moss biomonitoring technique has been applied to air pollution monitoring in South Albania. Moss samples were collected during the period of September–October 2010, and were analyzed for total concentration of the elements Al, As, Ba, Ca, Cd, Cr, Cu, Fe, K, Li, Mg, Mn, Na, Ni, P, Pb, Sr, V, and Zn by inductively coupled plasma–atomic emission spectrometry. Geographical distribution maps of the elements over the sampled territory were constructed using geographic information systems technology. Multivariate statistical analysis was applied to distinguish elements mainly of anthropogenic origin from those predominantly originating from natural sources. Four factors were identified: Factor 1 reflects wind-blown mineral particles or local emissions from industry (Al, As, Ba, Ca, Cr, Cu, Fe, Mn, Ni, V, Zn); Factor 2 is related to long-range atmospheric transport of elements or local emissions from industry (Cd, Pb); Factor 3 (Na, Mg) and Factor 4 (K) reflect the natural origin of elements as crustal, marine, and vegetation components.