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This research examined two questions: (1) What is the prevalence of self-injurious behavior (SIB) among college students, overall and by gender, academic level, and sexual orientation? (2) To what extent is SIB associated with different forms of substance use and other risk behaviors? A probability sample of 5,689 students completed an Internet survey on self-injury, mental health, and substance use. Past-year prevalence of SIB was 14.3%, with undergraduates significantly more likely than graduate students to engage in SIB. Drug use and frequent binge drinking were associated with higher rates of SIB. Among those who engaged in any SIB, those who used drugs had higher depression scores, higher prevalence of cigarette smoking, and higher rates of binge eating. In a multiple logistic regression model predicting SIB, depression, cigarette smoking, gambling, and drug use were significant predictors. Information about those at risk for SIB is critical for the design of prevention and intervention efforts as colleges continue to grapple with risky behaviors.