Food insecurity is associated with mental health outcomes among adults experiencing homelessness. Different theoretical explanations have emerged to account for the negative health outcomes among vulnerable populations. The neomaterial theoretical perspective suggests that nutritional deficiencies from experiencing food insecurity are related to negative health outcomes. Whereas, the psychosocial theoretical perspective indicates that perceived disadvantages or inability to cope emotionally (i.e. lower distress tolerance) from food insecurity leads to adverse health outcomes. Building on these theoretical perspectives, the purpose of the study was to determine whether fruit and vegetable consumption (as a measure of diet quality) or emotional distress tolerance act as potential links between food insecurity and poor physical and mental health among adults experiencing homelessness. Adults were recruited from six area shelters in Oklahoma City (N = 566) during July-August 2016. Data was collected via a self-administered questionnaire on a tablet computer. Self-rated poor health, depression, and post-traumatic stress disorder (PTSD) were regressed on food insecurity using logistic regressions. Indirect effects were assessed using bootstrapping methods outlined by Preacher and Hayes. In covariate-adjusted models, lower levels of distress tolerance, but not fruit and vegetable consumption, partially mediated the association between food insecurity and poor health (β = 0.28, [0.14, 0.44]), depression (β = 0.56, [0.33, 0.88]), and PTSD (β = 0.39, [0.22, 0.60]). Results suggest that experiencing food insecurity may lower the ability to withstand emotional distress and consequently contributes to negative health outcomes.