Efforts are underway to understand recent increases in emergency department (ED) use and to offer case management to those patients identified as high utilizers. Homeless Veterans are thought to use EDs for non-emergent conditions. This study identifies the highest users of ED services in the Department of Veterans Affairs and provides descriptive analyses of these Veterans, the diagnoses for which they were seen in the ED, and differences based on their homeless status. Homeless Veterans were more likely than non-homeless Veterans to have >10 visits in the 2014 calendar year (12% vs. <1%). Homeless versus non-homeless Veterans with >10 visits were more often male, <age 60, and non-married. Non-homeless Veterans with >10 ED visits were often treated for chest and abdominal pain, and back problems, whereas homeless Veterans were frequently treated for mental health/substance use. Tailored case management approaches may be needed to better link homeless Veterans with high ED use to appropriate outpatient care.