Crack cocaine (crack) dependence is a severe disorder associated with considerable morbidity and mortality, constituting a major public health problem in Brazil. The aim of this study was to improve understanding of the profile of treatment-seeking crack-dependent individuals. We recruited 65 crack-dependent individuals from among those seeking treatment at an outpatient clinic for alcohol and drug treatment in the city of São Paulo, Brazil. Assessments, conducted between August 2012 and July 2014, focused on sociodemographic characteristics, the pattern/history of crack use, treatment history, concomitant substance use disorders, psychiatric symptomatology, and impulsivity. In the study sample, males predominated, as did unemployment, homelessness, and low levels of education. On average, the participants had smoked crack for 10 years. Most had previously been treated for crack dependence. Concomitant DSM-IV diagnoses of dependence on other substances were common, dependence on tobacco and alcohol being the most prevalent. Participants presented significant psychiatric symptomatology and impulsivity, with nearly half of the sample presenting psychotic symptoms, 90% presenting depressive symptoms, and 80% presenting anxiety symptoms. Most treatment-seeking crack-dependent individuals in Brazil are living in extremely poor social conditions and are struggling with the severe, chronic, and comorbid features of this disorder.