Considerable research on the risks of obesity and chronic diseases has focused on the relationships between where people live, where they shop, and the types of food they purchase. Rarely have investigators used a national sample and explicitly addressed whether people use neighborhood food stores to purchase food. Even more rarely have previous studies accounted for the broader built environment characteristics in which people live, access resources, socialize, and shop for food. We examined whether the cross-sectional associations between availability of neighborhood convenience stores and supermarkets and self-reported household annual expenditures for snacks and beverages still held after including regional destination accessibility, availability and diversity of neighborhood destinations, and neighborhood street connectivity. Our study included 49,048 households in 2010, located in 378 metropolitan areas in the continental United States. Households purchased more snacks if they lived in neighborhoods with many convenience stores. Access to unhealthy food includes a consideration of geographic proximity. The broader built environment characteristics was associated with food purchase, although the magnitude was small.