The ergot alkaloids (EAs) are mycotoxins produced by several species of fungi in the genus Claviceps. In Europe, Claviceps purpurea is the most widespread species and it commonly affects cereals such as rye, wheat, triticale, barley, millets and oats. Food and feed samples used to estimate human and animal dietary exposure were analysed for the 12 main C. purpurea EAs: ergometrine, ergosine, ergocornine, ergotamine, ergocristine, ergocryptine (α- and β-isomers) and their corresponding –inine (S)-epimers. The highest levels of EAs were reported in rye and rye-containing commodities. In humans, mean chronic dietary exposure was highest in ‘Toddlers’ and ‘Other children’ with maximum UB estimates of 0.47 and 0.46 μg/kg bw per day, respectively. The 95th percentile exposure was highest in ‘Toddlers’ with a maximum UB estimate of 0.86 μg/kg bw per day. UB estimations were on average fourfold higher than LB estimations. Average acute exposure (MB estimations) ranged from 0.02 μg/kg bw per day in ‘Infants’ up to 0.32 μg/kg bw per day estimated in ‘Other children’. For the 95th percentile acute exposure, the highest estimate was for a dietary survey within the age class ‘Other children’ (0.98 μg/kg bw per day). Dietary exposure estimates for animals, assuming a mean concentration scenario, varied between 0.31–0.46 μg/kg bw per day in beef cattle and 6.82–8.07 μg/kg bw per day (LB–UB) in piglets, while exposure estimates assuming a high concentration scenario (95th percentile) varied between 1.43–1.45 μg/kg bw per day and 16.38–16.61 μg/kg bw per day (LB–UB) in the same species. A statistically significant linear relationship between the content of sclerotia and the levels of EAs quantified was observed in different crops (barley, oats, rye, triticale and wheat grains). However, the absence of sclerotia cannot exclude the presence of EAs as samples with no sclerotia identified showed measurable levels of EAs (‘false negatives’).