Objective: Existing literature on young adults' e-cigarette and polysubstance use focused on college students. This study examined the differences between college and noncollege groups on prevalence and patterns of e-cigarette and other substance use using data from a national survey. Participants: Adults aged 18-24 from the 2013-2014 Population Assessment of Tobacco and Health Study (n = 6,608). Methods: Independent sample t-tests and Chi-square tests were conducted to examine group differences. Results: Noncollege young adults had higher prevalence of cigarette, e-cigarette, and marijuana use; college students had higher prevalence of alcohol use. Among current e-cigarette users, college students had higher prevalence of polysubstance use of alcohol and marijuana. College students used e-cigarettes for socializing purposes more. Conclusions: Differences in prevalence and patterns of e-cigarette and other substance use between college and noncollege groups exist. Future interventions should target the social context of college life and reach out to noncollege young adults in workplaces.