Objective: Although criminal behavior in veterans has been cited as a growing problem, little is known about why some veterans are at increased risk for arrest. Theories of criminal behavior postulate that people who have been exposed to stressful environments or traumatic events and who report negative affect such as anger and irritability are at increased risk of antisocial conduct. Method: We hypothesized veterans with posttraumatic stress disorder (PTSD) or traumatic brain injury (TBI) who report anger/irritability would show higher rates of criminal arrests. To test this, we examined data in a national survey of N = 1,388 Iraq and Afghanistan war era veterans. Results: We found that 9% of respondents reported arrests since returning home from military service. Most arrests were associated with nonviolent criminal behavior resulting in incarceration for less than 2 weeks. Unadjusted bivariate analyses revealed that veterans with probable PTSD or TBI who reported anger/irritability were more likely to be arrested than were other veterans. In multivariate analyses, arrests were found to be significantly related to younger age, male gender, having witnessed family violence, prior history of arrest, alcohol/drug misuse, and PTSD with high anger/irritability but were not significantly related to combat exposure or TBI. Conclusions: Findings show that a subset of veterans with PTSD and negative affect may be at increased risk of criminal arrest. Because arrests were more strongly linked to substance abuse and criminal history, clinicians should also consider non-PTSD factors when evaluating and treating veterans with criminal justice involvement. (Contains 4 tables and 1 figure.)