The present work was conducted to obtain and highlight the first comprehensive baseline data on atmospheric deposition of trace elements and to evaluate the air quality in Georgia. A total of 120 moss samples were collected over accessible territories in Georgia in the period from 2014 to 2017. Hylocomium splendens (Hedw.) Schimp., Hypnum cupressiforme (Hedw.), and Pleurozium schreberi (Brid.) Mitt. moss species were analyzed by two complementary analytical techniques: instrumental neutron activation analysis and atomic absorption spectrometry. Concentrations of 41 elements in mg/kg were determined. The concentrations were compared with the corresponding values in the literature and are in a good agreement, except for the concentration of Mg, Al, K, Ca, Ti, and Fe, which were higher than those reported for other countries. The principal component and discriminant analyses were implemented to extract information about the similar geochemical features and to decipher the provenance of the studied elements. The analysis showed that a considerable association of crustal elements and the provenance of elements can be considered as a mixture of geogenic and anthropogenic sources. In addition, the influence of different latitudinal climate zones on the distribution of elements in the atmospheric deposition was observed. The enrichment factor shows considerable values for Th and Zr. The spatial distribution of the pollution load index identifies four zones (#12, 38, 53, and 64). The potential ecological risk index and the risk index were calculated and it does not pose significant risk except As and Cd. The data obtained can be used as the first dataset of metal characterization of air pollution in Georgia.