Background: Cardiovascular disease is the leading cause of death, and smoking cessation is a key component of secondary cardiovascular disease risk prevention efforts. Objectives: To examine the relationships between demographic, clinical and health factors, history and patterns of smoking, nicotine dependence, withdrawal symptoms, and willingness (i.e., readiness) to quit smoking after hospital discharge among adult Jordanian men who were cigarette smokers and were admitted to the hospital with a cardiovascular disease diagnosis. Methods: This cross-sectional study recruited 118 adult men smokers from three hospitals in Jordan during 2011. Data were collected using structured interviews and medical record abstraction. Results: The mean age of smokers was 50.7 (±6.7) years and they smoked at least one cigarette per day for an average of 28.8 years (±7.0). Currently they smoke an average of 28.9 (±8.0) cigarettes a day. About a quarter (24.6%, n = 29) had previously made a quit attempt that lasted at least 24 hours. Smokers were considered highly nicotine dependent if they had scores of > 6 (out of 10) on the Fagerström Test for Nicotine Dependence scale. The average nicotine dependence score was significantly higher in the high versus low nicotine dependence group (6.9 vs. 4.1). The number of cigarettes smoked daily was significantly higher in the high compared to the low nicotine dependence group (30.7 cigarettes vs. 23.4). Logistic regression showed smokers who had someone available to encourage quitting smoking "at least sometimes" were more likely to quit smoking after hospital discharge, and smokers who had sufficient personal income to support self were less likely to quit smoking after hospital discharge, while controlling for all other variables. Conclusions: The very high nicotine dependence of these men indicates that there is an urgent need for education, counseling and behavioral interventions, and pharmacological therapies, to achieve successful smoking cessation. Study findings lay the basis for development of appropriate smoking cessation programs in Jordan.