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Objectives. To assess the US incarcerated population's risk of exposure to per- and polyfluoroalkyl substances (PFASs). Methods. We assessed how many of the 6118 US carceral facilities were located in the same hydrologic unit code watershed boundaries as known or likely locations of PFAS contamination. We conducted geospatial analyses on data aggregated from Environmental Protection Agency databases and a PFAS site tracker in 2022 to model the hydrologically feasible known and presumptive PFAS contamination sites for nearly 2 million incarcerated people. Results. Findings indicate that 5% (∼310) of US carceral facilities have at least 1 known source of PFAS contamination in the same watershed boundary and that it is at a higher elevation than the facility; also 47% (∼2285) have at least 1 presumptive source. A minimum of 990 000 people are incarcerated in these facilities, including at least 12 800 juveniles. Exposure risks faced by incarcerated youths are disproportionately underassessed. Conclusions. The long-term impacts from potential exposures to PFAS are preventable and exacerbate health inequities among incarcerated populations. Widespread public attention to PFASs can be parlayed into broader environmental monitoring for imprisoned people. (Am J Public Health. 2024;114(5):501–510. https://doi.org/10.2105/AJPH.2024.307571) [ABSTRACT FROM AUTHOR]