Fine particulate matter 2.5 microns or less in diameter (PM2.5) is widely recognized to be a major public health concern. While ethnic/racial minority and lower socioeconomic status individuals in the US experience higher PM2.5 exposure, previous research on social disparities in PM2.5 exposure has not examined residents of federally-assisted public housing developments (PHDs). Here we present the first national-scale analysis of the relationship between outdoor PM2.5 exposure and PHD residency in the US, as well as exposure disparities within the population of households residing in PHDs. We integrated data on average annual PM2.5 concentrations (2011–2015) with US Department of Housing and Urban Development data on PHDs (2015), and socio-demographic information from the 2011–2015 American Community Survey. Results from multivariable generalized estimating equations indicated that PHD locations, units, and residents are significantly overrepresented in neighborhoods with greater PM2.5 exposure, after accounting for clustering, urbanization, and other socio-demographic factors. Additionally, significantly higher percentages of Black, Hispanic, disabled, and extremely low-income households reside in PHDs with greater PM2.5 exposure. Findings represent an important starting point for future research and emphasize the urgent need to identify gaps in environmental, public health, and housing policies that contribute to disproportionate air pollution exposures among PHD residents.