Background: Recommendations and policies, regarding the use of face coverings, have been instituted to control transmission of coronavirus disease 2019 (COVID-19). Understanding of psychosocial factors related to the use of face coverings within the context of COVID-19 is needed. This study aimed to conceptualize mask-wearing behavior among students using the Multi-theory Model (MTM) of behavior change. Methods: In October 2020, students (n = 595) enrolled in a large public southeastern US university were recruited to participate in a cross-sectional survey, using a valid and reliable instrument. Univariate, bivariate, and multivariate techniques described mask-wearing behavior and differentiated theoretical drivers of mask-wearing between individuals compliant and non-compliant with guidelines. Results: Compliant individuals reported significantly higher scores (P<0.05) for initiation and sustenance of mask-wearing, participatory dialogue, behavioral confidence, emotional transformation, practice for change, changes in the social environment, and significantly lower scores for disadvantage. Among multivariable models, all theoretical predictors exhibited significant relationships to their respective outcomes (initiation and sustenance). Specifically, MTM constructs explained approximately 35% of variance in initiation (R2 = 0.346, F(3,526) = 94.32, P<0.001) and 33% of variance in sustenance of mask wearing (R2 = 0.328, F(3,529) = 87.71, P<0.001) for compliant individuals. Behavioral confidence and emotional transformation exhibited the strongest relationships to initiation (ß = 0.403, P<0.001) and sustenance (ß = 0.450, P<0.001), respectively. Conclusion: Findings suggest a need to design educational programming based on the MTM to promote mask-wearing behavior among laggards who defy face mask guidelines, recommendations, and mandates.