Background: Marijuana use is increasing among adolescents and young adults. Long-term marijuana use magnifies the risk of a wide variety of behavioral, cognitive-emotional, and neurological problems, and can be a gateway to use of other drugs. In the present study, we investigated the cognitive-emotional and behavioral predictors of marijuana use. To this end, young Iranian adults answered questions based on an extended Theory of Planned Behavior (TPB) and related it to marijuana use. We hypothesized that cognitive-emotional and behavioral factors would predict intention to use marijuana, and that this, in turn, would predict actual consumption. Methods: A total of 166 young Iranian adults (mean age: 20.51 years; 15.7% females) attending a walk-in center for drug use took part in this cross-sectional study. Participants completed questionnaires covering sociodemographic information, frequency of marijuana use per week, along with questionnaires assessing the following dimensions of the TPB: attitude towards marijuana use, subjective norms, self-efficacy to resist marijuana use, environmental constraints, problem-solving skills, and behavioral intention for marijuana use. Results: Mean marijuana use was found to be 4.6 times/week. Attitude towards marijuana use, subjective norms, environmental constraints, and behavioral intention to use marijuana were positively correlated to each other and with marijuana use/week. In contrast, higher self-efficacy and problem-solving skills were associated with lower marijuana use/week. The multiple regression analysis showed that a positive attitude to marijuana use, lower self-efficacy in resisting its use, higher behavioral intention, and poorer problem-solving skills predicted actual use. Conclusion: The pattern of results suggests that dimensions of TPB can explain marijuana use among young Iranian adults self-admitted to a walk-in center for drug use. Specifically, poor problem-solving skills, low self-efficacy in resisting marijuana use, and positive labelling of its use appeared to be the best predictors of actual use. It follows that prevention programs aimed at improving problem-solving skills and raising self-efficacy, along with educational interventions aimed at highlighting the negative effects of marijuana might decrease the risk of its use among young adults in Iran.