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Certain types of athletic involvement may confer risk for substance use by college students. This study investigated whether motivational factors play a role in the relationship between athletic involvement and substance use. Intercollegiate athletes (n = 98) and exercisers (n = 120) were surveyed about substance use and motivation for athletic involvement. Athletes and exercisers who were extrinsically motivated had significantly higher rates of alcohol use than their intrinsically motivated counterparts. Results suggest that college students who are extrinsically motivated for involvement in physical activity/athletics—particularly those involved in team sports—may be in need of targeted prevention efforts.