Display omitted •Essential and toxic elements in raw milk were measured from four regions of Croatia.•As, Cd and Pb were detected above LOD in only 2.3–18.2% of milk samples, Hg in none.•Significant differences in Al, Ba, Se and Zn content were found among the regions.•Risk assessment showed low exposure of all elements in milk except for Cd. Concentrations of selected elements were measured in raw cow milk collected from four geographical regions in Croatia. The highest mean concentrations of Al, Ba, Fe and Zn were measured in milk from Central Croatia. Milk from the Croatian Littoral and Mountain region showed the highest mean content of Cd, Cr, Cu, Ni and Pb. The highest mean concentrations of As and Se were found in milk from Southern Croatia, while Mn had the highest values in Eastern Croatia. Mercury was not determined above the detection limit in any samples. Significant differences in the concentrations of Al, Ba, Se and Zn were found among the regions. A decrease in the Pb content was recorded compared to previous research in milk in Croatia. Estimation of the potential harmful effects of toxic and trace elements through milk consumption by comparing the established highest mean with toxicological limits showed low exposure with regard to Al, As, Ba, Cr, Cu, Hg, Fe, Ni, Se, Pb and Zn in adult populations in Croatia. The only exception was Cd concentrations in milk, which gave a higher contribution to toxicological limits, especially for consumers consuming greater quantities of milk per week.