This study identified demographic, clinical, and vocational rehabilitation-related correlates of long-term unemployment among 219 adults with severe mental illness. Fifty-one percent of the sample had been unemployed five or more years before enrollment. Older age, a diagnosis of psychosis, severity of negative symptoms, and more previous hospitalizations were all significantly related to long-term unemployment. Gender, race, education, substance disorder diagnosis, severity of negative symptoms, and vocational training experience were not. The findings underscore the relevance of clinical and neurocognitive impairments to long-term unemployment and point to the need to critically reevaluate the effectiveness of traditional vocational rehabilitation services.