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The current study examined the utility of behavioral measures of risk-taking propensity in the assessment of self-reported real-world risk-taking behaviors using a sample of 51 high-school-aged inner-city adolescents. Results indicated that performance on one behavioral measure, the balloon analogue risk task, accounted for unique variance in self-reported delinquency/safety risk behaviors as well as substance use risk behaviors, above and beyond that provided with demographics and self-report measures of risk-related constructs (i.e., impulsivity and sensation seeking). These results are discussed in relation to the potential utility of using a multimethod assessment approach for better understanding risk-taking vulnerability among adolescents.