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A multiyear water quality performance study of a bioretention rain garden located along a major urban transit corridor east of San Francisco Bay was conducted to assess the efficacy of bioretention rain gardens to remove pollutants. Based on data collected in three years between 2012 and 2017, polychlorinated biphenyls (PCBs) and suspended sediment concentrations (SSCs) were reduced (>90%), whereas total mercury (Hg), methylmercury (MeHg), and copper (Cu) were moderately captured (37%, 49%, and 68% concentration reduction, respectively). Anthropogenic microparticles including microplastics were retained by the bioretention rain garden, decreasing in concentration from 1.6 particles/L to 0.16 particles/L. Based on subsampling at 50- and 150-mm intervals in soil cores from two areas of the unit, PCBs, Hg, and MeHg were all present at the highest concentrations in the upper 100 mm in the surface media layers. Based on residential screening concentrations, the surface media layer near the inlet would need to be removed and replaced annually, whereas the rest of the unit would need replacement every 8 years. The results of this study support the use of bioretention in the San Francisco Bay Area as one management option for meeting load reductions required by San Francisco Bay total maximum daily loads, and provide useful data for supporting decisions about media replacement and overall maintenance schedules.