Background: Food insecurity is prevalent among college students in the United States and has been associated with mental health problems. However, the literature is not entirely consistent and is missing key aspects of mental health. Methods: Using cross-sectional data from the Health Minds Study (N = 96,379; September 2020–June 2021), we used multivariable logistic regression to examine associations between food insecurity and several aspects of mental health (i.e., depression, anxiety, languishing, perceived need, loneliness, self-injurious behaviors), adjusting for age, gender, race/ethnicity, financial distress, and parental education. Results: Food insecurity was associated with greater odds of having depression, anxiety, languishing, perceived need for help, loneliness, and self-injurious behaviors, adjusting for sociodemographic characteristics and markers of socioeconomic status. Conclusion: This study found evidence to suggest that food insecurity is related to poor mental health in a large sample of young adult college students in the United States, calling for targeted interventions.