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The authors tested how behavioral and emotional self-control are related to adolescent substance (tobacco, alcohol, and marijuana) use. Data were obtained from 489 middle school students and 602 high school students. Multiple indicators were developed for each domain of self-control, and confirmatory analyses were used to test the measurement structure of latent constructs. Results showed that the domains of behavioral self-control and emotional self-control were statistically distinct, and both were related to adolescent substance use. Structural modeling analyses indicated indirect effects for self-control constructs primarily through pathways to competence and recent events. In addition, poor behavioral control had a direct effect to deviant peer affiliations, and poor emotional control had a direct effect to coping motives for substance use. The results indicate that both types of self-regulation are relevant for adolescent substance use. Implications for prevention and treatment research are discussed.