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Premenstrual symptoms (PMS) may reduce smoking cessation success. Yet, little is known about the factors that may impact smoking cessation among women with elevated PMS, leaving little data to guide smoking cessation science and practice for this population. This cross-sectional study is a secondary analysis of data from laboratory studies focused on menstrual cycle effects and smoking. Premenopausal woman daily smokers (n = 157) completed self-report measures of tobacco dependence and other cessation-relevant factors (i.e., smoking cessation history, withdrawal during previous quit attempts, use of smoking cessation aids) as well as a measure assessing 3 domains of PMS—affective, water retention, and pain. After controlling for depression and race, affective PMS were associated with greater daytime tobacco dependence, withdrawal symptoms during most recent quit attempt, and number of smoking cessation aids used in past quit attempts (βs = .19–.28, ps < .05). Additionally, affective PMS were associated with increased odds of having used e-cigarettes during past quit attempts (odds ratio = 1.54, 95% confidence interval [1.06, 2.24]) after adjusting for depression and race. These results across different domains of PMS suggest that affective PMS may play a particularly important role in smoking cessation. Women with elevated affective PMS may be more inclined to try cessation aids and require special clinical attention to controlling tobacco withdrawal during quit attempts to increase success.