The sources of microplastics and other anthropogenic particles in freshwater are not well understood. The Greater Toronto Area, Canada's most populous urban area, offers a great study area for understanding the sources and pathways for microplastics to enter freshwater ecosystems. Here, we quantified and characterized microplastics and other anthropogenic particles from Lake Ontario surface waters and source waters (including stormwater runoff, agricultural runoff, and treated wastewater effluent) to better understand sources to the Great Lakes. Anthropogenic particle concentrations in lake samples were 0.8 particles L-1. In source waters, average concentrations were relatively higher in stormwater and wastewater, with 15.4 particles L-1 and 13.3 particles L-1, respectively, compared to 0.9 particles L-1 on average in agricultural runoff. Source waters revealed distinct signatures related to the morphologies of anthropogenic particles, e.g., fibers in wastewater. In addition, many upstream watershed characteristics were found to be significant predictors of anthropogenic particle concentration. Proximity to urban areas were positively correlated to anthropogenic particle concentrations. Future studies should focus on local source-apportionment to inform management and prevent further contamination of microplastics to freshwater ecosystems.