Using the 2016–2020 point-in-time homeless count data, this study investigates neighborhood characteristics associated with the levels of and changes in unsheltered homeless population density in Los Angeles. The results show that unsheltered homeless people in the study area are heavily concentrated in and around the city center, and in neighborhoods with greater access to shelters and lower socioeconomic status. Notably, neighborhoods closer to the city center experienced a relatively large increase in unsheltered homelessness during the study period, implying a persistent spatial concentration of unsheltered homelessness. The results consistently indicate that residential land share, Hispanic resident share, and the number of bridges in the baseline year are significant predictors of relative changes in unsheltered homelessness in subsequent years, whereas access to shelters and poverty rates are not. This study’s findings provide several important policy implications that could potentially help prevent and mitigate unsheltered homelessness.