Little is known about the relationship of food security (FS) status with mental health among students at minority-serving institutions. We aimed to elucidate the association of FS status with psychological distress and loneliness among full-time undergraduate students at a minority-serving institution. We used data from the National Collegiate Health Assessment III (n = 441). To assess FS, students responded to the USDA 6-item short form (range: 0–6) and responses were categorized as high (0), marginal (1) or low/very low (2–6) FS. The Kessler 6 scale assessed psychological distress (range: 0–24). The UCLA loneliness scale assessed loneliness (range: 3–9). Higher scores indicated higher psychological distress and loneliness. Using adjusted linear regression models, we examined the association of FS with psychological distress and loneliness. Compared to students with high FS (mean (SD): 9.4 (0.8)), students with marginal (11.4 (1.0); p < 0.05) or low/very low (11.8 (0.8); p < 0.01) FS had higher psychological distress scores. Compared to students with high FS (5.5 (0.3)), students with low/very low FS (6.0 (0.3); p < 0.05) had higher loneliness scores. Future studies should further explore these relationships using mixed methods, to provide complementary quantitative findings with the emic perspective of students and their experiences, which can inform programming to prevent and reduce food insecurity.