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Objectives In South Korea, there is limited information on nicotine dependence (ND) and its correlation with psychiatric disorders. Based on the National Epidemiologic Survey of Psychiatric Disorders in South Korea in 2006, we examined the relationship between the severity of tobacco smoking and mental disorders, paying specific attention to suicidal ideas, plans, and attempts. Methods A total of 6,510 adults underwent face-to-face interviews. The Korean version of the Composite International Diagnostic Interview (K-CIDI) was used to evaluate lifetime prevalence and correlates of mental disorders. According to the the severity of tobacco smoking, participants were grouped into never-smokers, ever-smokers, and ND. The frequencies of mental disorders and suicidal tendencies were analyzed among ND/ever-smokers. Multivariate logistic regression analysis was used to predict the odds ratios and significance levels among groups. Results Associations of ND with alcohol use disorder, mood disorder, anxiety disorder, pathological gambling, and suicidal tendencies were significant, even after controlling for demographic characteristics. Associations of most psychiatric disorders with smoking were stronger in females than in males. Conclusion ND is highly associated with alcohol use disorder, mood and anxiety disorders, pathological gambling, and suicidal tendencies. Interventions are needed in order to prevent the development of ND from regular smoking.