Urban air pollution is among the top 15 causes of death and disease worldwide, and a problem of growing importance with a majority of the global population living in cities. A important question for sustainable development is to what extent urban design can improve or degrade the environment and public health. We investigate relationships between satellite-derived estimates of nitrogen dioxide concentration (NO(2), a key component of urban air pollution) and urban form for 83 cities globally. We find a parsimonious yet powerful relationship (model R(2) = 0.63), using as predictors population, income, urban contiguity, and meteorology. Cities with highly contiguous built-up areas have, on average, lower urban NO(2) concentrations (a one standard deviation increase in contiguity is associated with a 24% decrease in average NO(2) concentration). More-populous cities tend to have worse air quality, but the increase in NO(2) associated with a population increase of 10% may be offset by a moderate increase (4%) in urban contiguity. Urban circularity ("compactness") is not a statistically significant predictor of NO(2) concentration. Although many factors contribute to urban air pollution, our findings suggest that antileapfrogging policies may improve air quality. We find that urban NO(2) levels vary nonlinearly with income (Gross Domestic Product), following an "environmental Kuznets curve"; we estimate that if high-income countries followed urban pollution-per-income trends observed for low-income countries, NO(2) concentrations in high-income cities would be ∼10× larger than observed levels.