OBJECTIVES: To determine whether history of traumatic brain injury (TBI) is associated with psychopathology, and, in particular, substance use disorder (SUD) in young adults with a history of athletic participation. DESIGN: Observational study. SETTING: University in the northeastern United States. PARTICIPANTS: A large (n = 534) and mixed sex (57% female) sample of varsity and club sport athletes older than 18 years. INTERVENTIONS: None. MAIN OUTCOME MEASURE: The Ohio State University Traumatic Brain Injury ID assessment and the Structured Clinical Interview for the diagnostic and statistical manual of mental disorders, fifth edition. RESULTS: Twenty-five percent of participants reported no history of head injuries, 32% reported 1 head injury, and 43% reported more than 1 head injury. Thirty-eight percent of participants had been diagnosed with 1 or more concussions. Twenty-eight percent of participants had a current psychiatric diagnosis and 49% had at least 1 lifetime diagnosis. Head injuries and concussions were significantly associated with the presence of lifetime psychiatric diagnosis and symptoms or diagnosis of alcohol or SUD. More head injuries were associated with symptoms of post-traumatic stress disorder. CONCLUSIONS: Higher number of self-reported head injuries and diagnosed concussions were associated with a lifetime history of psychopathology, and specifically, with alcohol and substance use disorders. These relationships are similar to those seen in the general population of adults. The relationships also raise several interesting questions about recovery from head injuries in young adult athletes.