Police violence is reportedly common among those diagnosed with mental disorders characterized by the presence of psychotic symptoms or pronounced emotional lability. Despite the perception that people with mental illness are disproportionately mistreated by the police, there is relatively little empirical research on this topic. A cross-sectional general population survey was administered online in 2017 to 1,000 adults in two eastern U.S. cities to examine the relationship between police violence exposure, mental disorders, and crime involvement. Results from hierarchical logistic regression and mediation analyses revealed that a range of mental health conditions are broadly associated with elevated risk for police violence exposure. Individuals with severe mental illness are more likely than the general population to be physically victimized by police, regardless of their involvement in criminal activities. Most of the excess risk of police violence exposure related to common psychiatric diagnoses was explained by confounding factors including crime involvement. However, crime involvement may necessitate more police contact, but does not necessarily justify victimization or excessive force (particularly sexual and psychological violence). Findings support the need for adequate training for police officers on how to safely interact with people with mental health conditions, particularly severe mental illness.