Abstract Background Food security is a severe problem in the United States. Few studies have examined its relationship with food shopping behaviors. Objective This study aimed to examine the association between food security and store-specific and overall food shopping among residents of low-income neighborhoods. Design We conducted a cross-sectional study. Participants/setting Five hundred twenty-seven households were recruited from two counties in South Carolina from November 2013 to May 2014, and 474 households were included in the final analysis. Main outcomes measures Food security was assessed using the 18-item US-Household Food Security Module questionnaire, and classified into three categories: high or marginal food security (FS), low food security (LFS), and very low food security (VLFS). Store-specific shopping behaviors including frequency, store type, and transportation were queried via in-person interview for the three most-frequented grocery stores. Distance from participants’ homes to their reported stores was calculated using Geographic Information Systems. Statistical analyses Multivariate linear regression for analyses of distance and frequency and multinomial/ordinary logistic regression for analyses of store type and transportation were used. Results Compared to FS participants, a significantly higher proportion of VLFS participants reported a convenience/dollar store as their most-frequented store (odds ratio OR 2.31, 95% CI 1.08 to 4.95) or a lack of transportation (OR 2.04, 95% CI 1.25 to 3.33). They also shopped less frequently (b=−.31, P =0.03) at their third most-frequented store and traveled fewer total miles for shopping (b=−4.71, P =0.04). In analyses considering all stores jointly, LFS participants had lower odds of shopping at both supermarkets and convenience/dollar stores (OR 0.44, 95% CI 0.21 to 0.91) compared to food-secure residents. Conclusions The current findings suggest that households with VLFS tend to shop more frequently in stores that have less-healthful options, such as convenience/dollar stores. These findings lend support to ongoing community and policy interventions aimed at improving food access among food-insecure populations.