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This study explores the role of substance use expectancies as mediators between the Dark Triad of personality, substance use, and substance use preferences. A sample of college students (M = 19.38, SD = 2.63, N = 207) completed an online questionnaire that assessed the Dark Triad traits, substance use history, substance preferences, and substance use expectancies. Three specific substance use expectancies—increased confidence, tension reduction, and cognitive enhancement—were shown to either partially or fully mediate the relationships between the Dark Triad and substance use behaviors and preference for certain substances of abuse. These findings may hold clinical implications for the treatment of substance use disorders and further the understanding of factors contributing to the etiology and progression of substance abuse and substance use disorders.