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Rural communities experience disproportionately high rates of food insecurity and diet-related chronic disease, yet limited research has examined how structural constraints shape food purchasing decisions. This study investigated how food insecurity and rural food environments are associated with the prioritization of food characteristics among low-income adults in rural South Carolina during the COVID-19 pandemic. A sample of 632 low-income adults in nine rural South Carolina counties from a cross-sectional survey (August 2020–July 2021) ranked the importance of food characteristics, including nutritional value, price, appearance, locally grown, and organically grown attributes. Associations between food insecurity, perceived ease of food access, food desert residence, and ranked priorities were examined using ordinal logistic, multinomial logistic, and rank-ordered logit models. Food insecurity was consistently associated with food choice priorities. Compared with food-secure respondents, those experiencing moderate or high food insecurity were significantly more likely to prioritize price and less likely to prioritize nutritional value across analytic approaches. Greater perceived ease of food access was associated with increased prioritization of nutrition and reduced emphasis on price. Residence in food desert areas was modestly associated with prioritizing affordability over nutritional value. Among rural adults, economic hardship and constrained food environments shape food purchasing priorities, often limiting the ability to prioritize nutrition. These findings highlight the central role of structural barriers in driving rural nutrition disparities and suggest that improving rural health will require policies that address both economic insecurity and access to affordable, healthy foods.