Background: Urban populations have grown globally alongside emerging simultaneous burdens of undernutrition and obesity. Yet, how heterogeneous urban environments are associated with this nutritional double burden is poorly understood. Objective: We aimed to determine: 1) the prevalence of the nutritional double burden and its components in urban, peri-urban, and rural areas of Bolivia; and 2) the association of residence in these areas with the nutritional double burden and its components. Design: We surveyed 3946 randomly selected households from 2 metropolitan regions of Bolivia. Census data and remotely sensed imagery were used to define urban, peri-urban, and rural districts along a transect in each region. We defined 5 nutritional double burdens: concurrent overweight and anemia among women of reproductive age (15-49 y), and children (6-59 mo), respectively; concurrent overweight and stunting among children; and households with an overweight woman and, respectively, an anemic or stunted child. Capillary hemoglobin concentrations were measured to assess anemia (women: hemoglobin <120 g/L; children: hemoglobin <110 g/L), and overweight and stunting were calculated from height, weight, and age data. Results: In multiple logistic regression models, peri-urban, but not urban residence, was associated with higher odds of concurrent overweight and anemia among children (OR: 1.8; 95% CI; 1.0, 3.2) and of households with an overweight woman and stunted child (1.8; 1.2, 2.7). Examining the components of the double burden, peri-urban women and children, respectively, had higher odds of overweight than rural residents [women (1.5; 1.2, 1.8); children (1.5; 1.0, 2.4)], and children from peri-urban regions had higher odds of stunting (1.5; 1.1, 2.2). Conclusions: Peri-urban, but not urban, residence in Bolivia is associated with a higher risk of the nutritional double burden than rural areas. Understanding how heterogeneous urban environments influence nutrition outcomes could inform integrated policies that simultaneously address both undernutrition and obesity.