It is well-known that consumption of nutrient-rich foods, especially fruits and vegetables, are low among food insecure populations. While cost is an important reason for these inadequate diets, underlying factors such as poor food purchase and management behaviors, and low levels of psychosocial factors that motivate dietary improvements, may exacerbate food insufficiency among the food-insecure. In this analysis, we examine these underlying factors across food-secure and food-insecure populations in Texas. Data on self-reported food insecurity, dietary practices, behaviors related to food purchase and management, and psychosocial factors related to food were obtained from a survey administered to a convenience sample of SNAP-eligible adults (n = 1,171) ages 18 and older, drawn from multiple low-income areas across the state of Texas in 2018 over two survey rounds. Mixed linear regression models adjusting for zip code as a random effect were used to compare mediators of diet across food-insecure and food-secure participants. Using the binary categories defined by the U.S. Household Food Security Survey Module scale 753 participants (64.3% of the sample collected) were classified as food insecure. Food insecure participants had notably unhealthier diet profiles, with significantly lower (p < .001) frequency and average serving size of fruit and vegetable consumption. They were also less likely to use food labels to make food choices (p < .001), and to cook a meal at home (p = .008). In contrast, differences across food secure and food insecure households in planning meals before going shopping, and making lists were much smaller. Finally, levels of various psychosocial precursors of healthy eating were also lower among food insecure participants, including self-efficacy for healthy eating (p = .014), self-efficacy to plan meals with vegetables (p = .048), and stage of change of fruit and vegetable consumption (p < .001). Overall, eating habits, specific food procurement and preparation practices, and levels of psychosocial precursors of healthy eating are significantly poorer among food insecure populations compared with food-secure low-income participants. Our results point to specific behaviors that can be targeted in educational and skill building interventions seeking to address poor dietary practices among the food insecure.