The association between cerium status and risk of first acute myocardial infarction (AMI) was examined in a case-control study in 10 centres from Europe and Israel. Cerium in toenails was assessed by neutron activation analysis in 684 cases and 724 controls aged 70 years or younger. Mean concentrations of cerium were 186 and 173 μg/kg in cases and controls, respectively. Cerium was positively associated with low socio-economic status, smoking, mercury, zinc and scandium (p 0.001). Cases had significantly higher levels of cerium than controls after adjustment for age and centre (case-control ratio 1.074; 95% CI 1.002–1.151) and increased in further adjustment for other cardiovascular risk factors 1.085; 95% CI 1.025–1.149. The risk after adjustment for age and centre was higher with increasing cerium levels (p for trend = 0.02). After adjustment for BMI, history of hypertension, smoking, alcohol intake, diabetes, family history of CHD, β-carotene, lycopene, α-tocopherol, selenium, mercury and scandium, the OR for the highest quintile was 1.43 (95% CI 0.85–2.41; p-trend 0.08). When we applied this same model in non-smokers the odds ratios in the 4th and 5th quintiles of cerium as compared with the lowest were 2.09 (95% CI 1.05–4.16) and 2.81 (95% CI 1.21–6.52), respectively, p-trend 0.011. Our results suggest that toenail cerium levels may be associated with an increased risk of AMI, but more research is warranted to shed further light and fully understand the plausibility and public health implications of these findings.