Using intercept surveys, we explored demographic and socioeconomic factors associated with food purchasing characteristics of supermarket shoppers and the perceptions of their neighborhood food environment in urban Cape Town. Shoppers (N = 422) aged ≥18 years, categorized by their residential socioeconomic areas (SEAs), participated in a survey after shopping in supermarkets located in different SEAs. A subpopulation, out-shoppers (persons shopping outside their residential SEA), and in-shoppers (persons residing and shopping in the same residential area) were also explored. Fruits and vegetables (F&V) were more likely to be perceived to be of poor quality and healthy food not too expensive by shoppers from low- (OR = 6.36, 95% CI = 2.69, 15.03, p < 0.0001), middle-SEAs (OR = 3.42, 95% CI = 1.45, 8.04, p < 0.001) compared to the high-SEA shoppers. Low SEA shoppers bought F&V less frequently than high- and middle-SEA shoppers. Purchase of sugar-sweetened beverages (SSBs) and snacks were frequent and similar across SEAs. Food quality was important to out-shoppers who were less likely to walk to shop, more likely to be employed and perceived the quality of F&V in their neighborhood to be poor. Food purchasing characteristics are influenced by SEAs, with lack of mobility and food choice key issues for low-SEA shoppers.