Instrumental neutron activation analysis in combination with the method of moss biomonitoring for the assessment of atmospheric deposition of heavy metals and other elements was applied for the first time in the Ryazan Region in Russia. Concentrations of 42 macro, micro and trace elements in 63 moss samples (Hylocomium splendens and Pleurozium schreberi, as well as Hypnum cupressiforme, Sciuro-hypnum sp., Plagiothecium sp. and Ptilium sp.), collected on a relatively uniform grid in the study area, were determined. On the basis of analytical results using GIS technologies, maps of the spatial distribution of heavy metals and other toxic elements were constructed for the Ryazan region. The method of multivariate statistical analysis (factor analysis) was used to identify the main sources of pollution—large industrial facilities located in this region. The obtained results were included in the Atlas of Atmospheric Deposition of Heavy Metals, which is published by the UN Commission on Long-Range Transboundary Air Pollution (UNECE ICP Vegetation).