We identified correlates of unsheltered status among Veterans experiencing homelessness and described distinct subgroups within the unsheltered homeless Veteran population using data from a screening instrument for homelessness that is administered to all Veterans accessing outpatient care at a Veterans Health Administration (VHA) facility. Correlates of unsheltered homelessness included male gender, white race, older age, lower levels of VHA eligibility, substance use disorders, frequent use of VHA inpatient and infrequent use of VHA outpatient services, and residing in the West. We identified six distinct subgroups of unsheltered Veterans; the tri-morbid frequent users represented the highest need group, but the largest group was comprised of Veterans who made highly infrequent use of VHA healthcare services. Differences between sheltered and unsheltered Veterans and heterogeneity within the unsheltered Veteran population should be considered in targeting housing and other interventions.