The Post-Concussion Symptom Scale (PCSS) measures cognitive, sleep-arousal, physical, and affective symptoms that typically follow sport-related concussion (SRC). Mental health symptoms are associated with postconcussion-like symptoms, regardless of concussion status. This study examined whether mental health or SRC history had a stronger relation with symptom reporting and investigated the association between PCSS scores and perceived academic functioning. College students (N = 554) reported SRC history, current anxiety and depression symptoms, and academic self-efficacy. Participants were divided into healthy, SRC, anxiety, and depression groups then compared on individual symptom endorsement, symptom severity (total score and subscales), and academic self-efficacy. Healthy participants had lower endorsement rates than the anxiety/depression groups on all PCSS items (ps < .001) but vomiting, and lower symptom severity on each PCSS subscale and the total score (ps < .001, d range = .89 to 1.86). The healthy and SRC groups differed on only one item (i.e., trouble falling asleep, p < .001), one subscale (sleep-arousal, p < .01, d = .33), and the total score (p < .01, d = .27), with subtly greater severity in the SRC group. The cognitive subscale had the strongest relation with academic self-efficacy for every group (rho range = −.23 to −.36). Larger differences emerged when comparing healthy participants to those screening positive for anxiety/depression than those with an SRC history, indicating current mental health has a stronger relation with postconcussion-like symptoms than remote SRCs. Cognitive symptoms were strongly associated with perceived academic ability. In college students with a history of SRC, mental health symptoms may explain lasting symptoms and necessitate intervention for academic performance.