Rooftops are both a source of and a pathway for contaminated runoff in urban environments. To investigate the importance of particle-associated contamination in rooftop runoff, particles washed from asphalt shingle and galvanized metal roofs at sites 12 and 102 m from a major expressway were analyzed for major and trace elements and PAHs. Concentrations and yields from rooftops were compared among locations and roofing material types and to loads monitored during runoff events in the receiving urban stream to evaluate rooftop sources and their potential contribution to stream loading. Concentrations of zinc, lead, pyrene, and chrysene on a mass per mass basis in a majority of rooftop samples exceeded established sediment quality guidelines for probable toxicity of bed sediments to benthic biota. Fallout near the expressway was greater than farther away, as indicated by larger yields of all contaminants investigated, although some concentrations were lower. Metal roofing was a source of cadmium and zinc and asphalt shingles a source of lead. The contribution of rooftop washoff to watershed loading was estimated to range from 6 percent for chromium and arsenic to 55 percent for zinc. Estimated contributions from roofing material to total watershed load were greatest for zinc and lead, contributing about 20 and 18 percent, respectively. The contribution from atmospheric deposition of particles onto rooftops to total watershed loads in stormwater was estimated to be greatest for mercury, contributing about 46 percent.