Objectives: To explore the association of neuroticism with the metabolic syndrome, separate components of the metabolic syndrome, and the number of components of metabolic syndrome an individual possesses. To examine the extent to which any associations are accounted for by socio-demographic factors, health behaviours, and cognitive ability. Method: Participants were 4,208 men drawn from the Vietnam Experience Study. From military archives, and a later telephone interview and psychological and medical examination, socio-demographic, health behaviour, cognitive ability, neuroticism, and health data were collected. Neuroticism and cognitive ability were assessed with standardised tests during the medical examination. Presence of the metabolic syndrome was based on: body mass index; fasting blood glucose or a diagnosis of diabetes; high blood pressure or taking antihypertensive medication; HDL cholesterol; and triglyceride levels. Results: Neuroticism was positively associated with the occurrence of the metabolic syndrome and several of its components in both age-, and socio-demographic- and health behaviour-adjusted analyses. Many associations were accounted for by individual difference in cognitive ability. Neuroticism was robustly associated with the number of components of the metabolic syndrome after adjustment. Conclusions: Individuals with higher neuroticism scores had a higher prevalence of the metabolic syndrome, and a larger number of its components. On the whole, differences in cognitive ability appeared to partially mediate, the relationship between neuroticism and the metabolic syndrome