Rainfall runoff samples were collected from streets, parking lots, roofs, driveways, and lawns. These five source areas are located in residential, commercial, and industrial land uses in Madison, Wisconsin. Solids, phosphorus, and heavy metals loads were determined for all the source areas using measured concentrations and runoff volumes estimated by the Source Load and Management Model. Source areas with relatively large contaminant loads were identified as critical source areas for each land use. Streets are critical source areas for most contaminants in all the land uses. Parking lots are critical in the commercial and industrial land uses. Lawns and driveways contribute large phosphorus loads in the residential land use. Roofs produce significant zinc loads in the commercial and industrial land uses. Identification of critical source areas could reduce the amount of area needing best-management practices in two areas of Madison, Wisconsin. Targeting best-management practices to 14% of the residential area and 40% of the industrial area could significantly reduce contaminant loads by up to 75%.