Radioactive (radon) groundwaters are highly valued among mineral waters for their healing effects. Between 2005 and 2015, a large exploratory event for prospecting and documenting radon water springs took place in the crystalline area of Lugicum (Bohemian Massif) under Czech–Polish cooperation. For these purposes, an exploration method was developed as a combination of GIS (ArcMap 9.1–10.2) area preparation followed by field radiohydrogeochemical mapping at a scale of 1:10,000. The gamma indication method was optimized and used for the selection of water samples. A total of 2354 water sources were examined. Radon activity concentrations were measured at 660 sources found throughout the territory. Of those, 111 sources exhibited 222Rn activity above 1500 Bq/L and, thus, were categorized as sources of mineral radioactive waters according to Czech legislation. The highest 222Rn activity was found in the Michael spring near Nové Město pod Smrkem (up to 6237 Bq/L 222Rn). Many discovered sources with high balneological potential are significant and, therefore, are quickly becoming popular among the public.