While Value-Belief-Norm (VBN) theory has been widely applied to various populations, it has seldom been tested on college students. This study extends VBN theory to examine what socio-psychological factors influence sustainability behaviors among university students. Undergraduate students are an interesting and novel population, as they are still forming their values and beliefs, and therefore may be more open to engage in sustainability efforts. This study assessed five sustainability behaviors: (a) support for political candidates who say they will strengthen environmental policies, (b) recycling, (c) electricity use, (d) food selection, and (e) transportation choices. Findings support the notion that one’s values matter in environmental decision-making, but that different values are associated with different behaviors. Those who adhere to biospheric and altruistic values were more likely to engage in a range of sustainability behaviors whereas those who adhere to egoistic values were less likely to engage in most behaviors. Those who adhere to traditional or openness to change values showed mixed results. We discuss the theoretical application, practical recommendations for behavior change campaigns, and offer suggestions for future research.