Although there has been considerable research on consumers’ opinions about sustainable foods and purchasing behaviors, the experience of university students remains unclear. This study aims to characterize university students’ perceptions of the importance of sustainable foods and determine the relationship between perceptions and the frequency of purchasing sustainable foods. In a non-random sample of university students, a cross-sectional, online survey determined students’ perceptions of the importance of locally grown food and sustainable foods, and the self-reported frequency of purchasing sustainable foods. Multivariate binary logistic regression was conducted. Survey respondents (n = 1858; 71% female; 80% domestic enrolled; 43% aged 18–24 y; 38% food insecure) perceived locally grown food (77%) and sustainable food (84%) as important, and 68% reported buying sustainable foods frequently. Students who purchased sustainable foods frequently were more likely to be female, older and food insecure, and also were significantly more likely to perceive sustainable foods as important (OR: 7.317; 95%-CI: 5.538–9.667; SE: 0.142; p < 0.001). Our results demonstrate that university students perceive sustainable foods as important and a relationship between perceptions and actions for purchasing sustainable foods is evident. Our results should inform the development of strategies within universities aligned with the United Nations Sustainable Development Goals, including improving access to locally grown and sustainable foods on campus to reflect student preferences, particularly for food insecure students.