Background: Alcohol use and nonsuicidal self-injury (NSSI) appear to share a conceptual overlap in functions (e.g., tension reduction). Alcohol use has been identified as a risk factor for NSSI, and higher rates of alcohol use have been documented among those with NSSI history. Aims: This study examined whether NSSI-related alcohol expectancies affect relations between NSSI and alcohol use. Method: Participants were 367 college students (73% female) asked to complete an online survey about their drinking behavior and lifetime NSSI. Results: NSSI and alcohol use were highly prevalent in this sample: 56% endorsed lifetime NSSI and 74% endorsed current alcohol use. Of note, 43% (n = 147) endorsed both behaviors. Positive NSSI-related alcohol expectancies showed a significant association with lifetime NSSI. In addition, positive NSSI-related alcohol expectancies were associated with more frequent drinking behavior for individuals with a history of NSSI, particularly those who had engaged in two or more methods of lifetime NSSI. Conclusion: Alcohol use and NSSI represent high-risk behaviors commonly employed to regulate unwanted affective states. Interventions targeting substance use and/or NSSI may consider assessing positive NSSI and substance use expectancies, as the presence of these beliefs suggests a higher risk profile.