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Several studies have documented that more deprived populations tend to live in areas characterized by higher levels of environmental pollution. Yet, time trends and geographic patterns of this disproportionate distribution of environmental burden remain poorly assessed, especially in Europe. We investigated the spatial and temporal relationship between ambient air nitrogen dioxide (NO2) concentrations and socioeconomic and demographic data in four French metropolitan areas (Lille in the North, Lyon in the center, Marseille in the South, and Paris) during two different time periods. The geographical unit used was the census block. The dependent variable was the NO2 annual average concentration (μg/m(3)) per census block, and the explanatory variables were a neighborhood deprivation index and socioeconomic and demographic data derived from the national census. Generalized additive models were used to account for spatial autocorrelation. We found that the strength and direction of the association between deprivation and NO2 estimates varied between cities. In Paris, census blocks with the higher social categories are exposed to higher mean concentrations of NO2. However, in Lille and Marseille, the most deprived census blocks are the most exposed to NO2. In Lyon, the census blocks in the middle social categories were more likely to have higher concentrations than in the lower social categories. Despite a general reduction in NO2 concentrations over the study period in the four metropolitan areas, we found contrasting results in the temporal trend of environmental inequalities. There is clear evidence of city-specific spatial and temporal environmental inequalities that relate to the historical socioeconomic make-up of the cities and its evolution. Hence, general statements about environmental and social inequalities can be made.