Impacts of surface runoff to aquatic species are an ongoing area of concern. Tire and road wear particles (TRWP) are a constituent of runoff, and determining accurate TRWP concentrations in sediment is necessary in order to evaluate the likelihood that these particles present a risk to the aquatic environment. TRWP consist of approximately equal mass fractions of tire tread rubber and road surface mineral encrustations. Sampling was completed in the Seine (France), Chesapeake (U.S.), and Yodo-Lake Biwa (Japan) watersheds to quantify TRWP in the surficial sediment of watersheds characterized by a wide diversity of population densities and land uses. By using a novel quantitative pyrolysis-GC/MS analysis for rubber polymer, we detected TRWP in 97% of the 149 sediment samples collected. The mean concentrations of TRWP were 4500 (n = 49; range = 62-11 600), 910 (n = 50; range = 50-4400) and 770 (n = 50; range = 26-4600) μg/g d.w. for the characterized portions of the Seine, Chesapeake and Yodo-Lake Biwa watersheds, respectively. A subset of samples from the watersheds (n = 45) was pooled to evaluate TRWP metals, grain size and organic carbon correlations by principal components analysis (PCA), which indicated that four components explain 90% of the variance. The PCA components appeared to correspond to (1) metal alloys possibly from brake wear (primarily Cu, Pb, Zn), (2) crustal minerals (primarily Al, V, Fe), (3) metals mediated by microbial immobilization (primarily Co, Mn, Fe with TOC), and (4) TRWP and other particulate deposition (primarily TRWP with grain size and TOC). This study should provide useful information for assessing potential aquatic effects related to tire service life.