Naturally occurring radionuclides were studied through the Bayer process by calculating their mass flows. Aluminium of Greece (AoG) provided sample materials and plant data from several process stages. Measurements of radionuclide concentrations were carried out by gamma-ray spectroscopy. The performed measurements show that in the specific case of the AoG plant, the majority of the natural radionuclides were introduced with karst bauxites, which showed higher activity concentrations for nuclides compared to lateritic bauxites. Most of these nuclides accumulated in the bauxite residue, while only a minor portion of uranium isotope U-238 was found in alumina, corresponding to 3% of its input value. Uranium was observed to partially dissolve in the process liquors similarly to K-40, whereas the latter was not associated with aluminium hydroxide. All the materials studied in the current research work had radionuclide concentrations well below the exemption limits set by EURATOM Basic Safety Standard, indicating that these naturally occurring radionuclides do not pose a radiological hazard for workers of the AoG plant or the public.