Diet is a primary source of pollutant exposure. Given children's vulnerability to their effects, this study assessed dietary intake of metals/metalloids and different persistent organic pollutants in children in Tarragona (Spain), compared it with the health-based guideline values (HBGV), and identified the main dietary sources. The analysis included 533 preschoolers and 443 primary school children from the EPINED and ECLIPSES studies. Dietary intake of cadmium (Cd), methylmercury (MeHg), lead (Pb), inorganic arsenic (inAs), polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), dioxin-like polychlorinated biphenyls (DL-PCBs), and non-dioxin-like polychlorinated biphenyls (NDL-PCBs) was estimated using validated food frequency questionnaires and a database from the Catalan Agency for Food Safety. Preschoolers and primary school children exceeded the relevant reference value for InAs and DL-PCBs. Only preschoolers exceeded the limit for MeHg and PCDD/Fs. Cd, Pb, and NDL-PCBs intakes did not exceed the limits in either age group. Salted cereals/potatoes were the main source of InAs; fish for MeHg and DL-PCBs; and milk/yogurt for PCDD/Fs, followed by white fish in preschoolers and fatty fish in primary school children. The findings highlight that dietary exposure to some pollutants poses a significant risk to these children, emphasizing the need for public health policies to reduce pollutants in their diets.