Research demonstrates that smoking is highly correlated with, and a cause of, head and neck cancer and Chronic Obstructive Pulmonary Disease (COPD). Although the prevalence of smoking has declined since 1965, a significant proportion of the population continue to smoke. In addition to smoking being a cause of cancer and COPD, smoking has also been implicated in the progression of disease-related symptoms, diminished treatment outcome, and recurrence of disease. Previous research demonstrates that approximately 70% of individuals with COPD continue to smoke as compared to approximately 30% of individuals with head and neck cancer. Most of the studies have focused on demographic, smoking, disease severity and treatment variables, with little attention to psychosocial variables. Whereas demographic variables are stable variables which cannot be reversed, psychosocial variables are important to investigate not only because they may serve as obstacles to smoking cessation, but also, because interventions exist which would allow health professionals to intervene and increase smoking cessation success. This study investigated psychosocial predictors of smoking cessation in the head and neck cancer and COPD populations. One- hundred and three participants completed a semi-structured interview of their smoking history and two self-report questionnaires, the Profile of Mood States and the Social Problem-Solving Inventory - Revised. Fifty-four and 49 participants were diagnosed with COPD and with head and neck cancer, respectively. Approximately 31% of individuals with COPD and 26% of individuals with head and neck cancer were current cigarette smokers, resulting in 29% of the combined sample currently smoking cigarettes. A logistic regression found that marital status, alcohol use, and depression predicted smoking status. The smoking history, problem solving, and anger variables did not predict smoking status. In the final model, approximately 25% of the variance was accounted for. A response operating characteristics analysis yielded a model with 71% sensitivity, 68% specificity, and an overall classification rate of 70%. The results suggest that for individuals who are diagnosed with either head and neck cancer or COPD, and who report some distress, psychosocial treatment that addresses alcohol use and that is geared toward decreasing depression may help these individuals quit smoking.