Radiation Protection Unit of the Institute for Medical Research and Occupational Health in Zagreb has been conducting systematic investigations of radioactive contamination of the Croatian environment by anthropogenic fission products as well as by naturally occurring radioactive material (NORM) since 1963. Several critical sites in Croatia were identified for NORM, that is, for slag and ash repositories from coal-fired power plants and phosphogypsum repository from a mineral fertilizer production plant. As the coals and phosphate ores contain naturally occurring radionuclides, especially the members of the uranium and thorium radioactive chains, utilising these materials in various industries only enhances their natural radioactivity in residual waste. Consequently, the resulting activity concentrations of natural radionuclides in waste material could be several times higher than in the adjacent soil. These deposited materials pose permanent risk of radiation exposure due to the long physical half-life of natural radionuclides (e.g., T 1/2 = 1600 years for 226Ra). Results of scientific investigations related to natural radioactivity are used in the recovery of slag and ash repositories and landfills, as well as in establishing regulatory criteria targeting import of coal and phosphate ores. In consequence, recently measured activity concentrations of natural radioactivity in imported materials used nowadays in coal-fired power plants are significantly lower than in previously used raw materials. Therefore, slag and ash can be used as additive materials in cement production.