The results of multifaceted studies using multiscale methods of mapping and assessment of the natural radioactivity of actual rare-metal ores, and non-metallic raw materials from the Kola and Karelian regions are presented. The thorium specialization was found to be predominant among nepheline-syenite complexes productive in rare metals, and the thorium-uranium specialization prevailed among carbonatite and granitepegmatite complexes. The distribution patterns of natural radionuclides in ore bodies, the mineral forms of their concentration, and their radioecological significance in assessing the quality of the studied types of raw materials and handling them during mining and processing were determined. For the territory of the City of Murmansk, mainly represented by outcrops of the Precambrian basement, the parameters of radon ‘respiration’, areas of abnormal concentrations, and their confinement to fault zones were revealed in the geotectonic base map. The effectiveness of the combined use of the results of radio-geochemical mapping and radiation-hygienic surveys of settlements in the regions is demonstrated.