Ecological studies often use supermarket location as a proxy measure of the food environment. In this study, we used data on sales at a leading mainstream supermarket chain to explore how area-level supermarket use is associated with overweight and obesity in English adults. Sales data were aggregated to local authority level and joined to a national dataset describing self-reported height and weight and fruit and vegetable consumption. Regression models showed a modest association between higher levels of unhealthy food sales relative to health food sales and increased odds of being overweight and obese. Although effect sizes were small, they persisted after adjustment for area-level deprivation. Supermarket sales data provide additional understanding in the study of food environments and their impact on increasing weight status. Future health policies should consider using ‘big data’ combined with other research methods to address the increasing consumption of unhealthy and highly processed foods.