The objective of this paper is to model determinants of intraurban variation in ambient concentrations of nitrogen dioxide (NO2) in Toronto, Canada, with a land use regression (LUR) model. Although researchers have conducted similar studies in Europe, this work represents the first attempt in a North American setting to characterize variation in traffic pollution through the LUR method. NO2 samples were collected over 2 wk using duplicate two-sided Ogawa passive diffusion samplers at 95 locations across Toronto. Independent variables employed in subsequent regression models as predictors of NO2 were derived by the Arc 8 geographic information system (GIS). Some 85 indicators of land use, traffic, population density, and physical geography were tested. The final regression model yielded a coefficient of determination (R2) of .69. For the traffic variables, density of 24-h traffic counts and road measures display positive associations. For the land use variables, industrial land use and counts of dwellings within 2000 m of the monitoring location were positively associated with NO2. Locations up to 1500 m downwind of major expressways had elevated NO2 levels. The results suggest that a good predictive surface can be derived for North American cities with the LUR method. The predictive maps from the LUR appear to capture small-area variation in NO2 concentrations. These small-area variations in traffic pollution are probably important to the exposure experience of the population and may detect health effects that would have gone unnoticed with other exposure estimates.