Background: Quit attempts are very essential in population-based smoking cessation. Little is known about the correlates of making a quit attempt of smoking in Bangladesh. We aimed to examine correlates of making a quit attempt of smoking among adults in Bangladesh. Methods: We used data from the 2009 Global Adult Tobacco Survey, Bangladesh. A total of 2217 adult current smokers (2141 males and 76 females) aged 15 years and older who participated in the survey were included. We compared socio-demographic, behavioral, motivational, knowledge and attitudes towards smoking, quitting methods utilized, use of social media to quit smoking, and environmental characteristics of current smokers who made an attempt to quit with those who made no quit attempt during the previous 12 months of the survey. We applied multivariable logistic regression models for analyzing the data. Results: Among the 2217 current smokers, 1058 (47.72%) made attempt to quit. We found respondents who smoked their first cigarette within 6 to 30 min of waking up were more likely to make an attempt to quit than those who smoked their first cigarette within 5 min of waking. Moreover, among daily current smokers who smoked 10–19 manufactured cigarettes per day were less likely to make a quit attempt. We also found intention to quit smoking, smoking rules inside the home, and exposure to anti-smoking advertisements as significant correlates of making a quit attempt of smoking among adults in Bangladesh. Conclusions: Policymakers should consider our findings when implementing tobacco control programs in Bangladesh.