These data represent a one-time synoptic survey of sampled soils, pavement dust, and stream sediment in 10 urban watersheds in three regions of the United States (Pacific Northwest, northeast, and southeast) to evaluate sources of sediment and two groups of common urban contaminants: polycyclic aromatic hydrocarbons (PAHs) and metals. Analyses of samples from six of the watersheds included fallout radionuclides to facilitate identification of sediment sources to the streams. Scripts used in R to test selected explanatory variables for the urban contaminants using Generalize Additive Models (GAMs) are included. The data release also includes Geographic Information System (GIS) spatial layers that were developed for the sediment sampling locations, the boundary of each associated watershed, and extents of parking lots identified as sealed or unsealed. These data were used to estimate area of sealed and unsealed pavement, both parking lots and driveways in residential neighborhoods in each watershed. The percentage of the watershed that was sealed pavement and the percentage of the sediment sample from pavement dust were used as explanatory variables in statistical models of PAH and metal concentrations in the streams. This data release includes two child items: 1) 4 data files containing the metals and PAH concentration data, radionuclide activity data, and pavement mapping statistics; a data dictionary describing the attributes in each data file; and R scripts and input files used for the GAM modeling; and 2) 3 GIS layers representing the sediment sampling locations, the associated watershed boundaries, and the parking lot aerial extents.