Objective: To compare persons who report that they never wear a seat belt while driving or as a passenger with those who do in a nationally representative sample in the United States. Our guiding hypothesis is that failure to wear a seat belt is part of an antisocial behavior spectrum. Methods: Using public-use data from the 2010 National Survey on Drug Use and Health, this study employed binary logistic regression with adjustments for complex survey sampling to assess relationships between never wearing a seat belt and sociodemographic variables, antisocial behaviors, substance abuse and co-occurring problems, and criminal justice system contact. Results: Individuals who do not wear seat belts are younger, more likely to be male, less likely to be African American or Hispanic, have incomes of less than $75,000, and be a high school or college graduate. After controlling for the effects of age, gender, race, income, education, and population density, individuals reporting that they never wear a seat belt while driving or as a passenger are more likely to report using alcohol and drugs (adjusted odds, 1.61e2.56), committing antisocial behaviors including felony offenses (adjusted odds, 2.13e3.57), and possess a dual diagnosis (adjusted odds, 1.62e1.73). Conclusions: Findings indicate that non-seat belt use is convergent with a spectrum of serious antisocial behavior and comorbid psychological distress. Importantly, results suggest that standard seat belt use policies and campaigns may not be effective for non-seat belt using individuals and a targeted approach may be needed.