We sought to extend previous research that demonstrates reduced neurometabolite concentrations during the chronic phase of pediatric traumatic brain injury (TBI) in children injured during early childhood. We hypothesized that young children with TBI in the chronic phase post-injury would have lower N-acetyl aspartate (NAA) metabolite concentrations in gray and white matter in comparison to controls. We also hypothesized that metabolite levels would be correlated with acute TBI severity and neurobehavioral skills. Ten children with a history of TBI between the ages of 3 and 6 years were compared to an age, gender, and race-matched group of 10 children with a history of an orthopedic injury (OI). Children completed neurobehavioral testing at 12 months post-injury. Proton magnetic resonance (MR) spectroscopy was completed at least 12 months post-injury when the children were 6-9 years old. Groups were compared on metabolite concentrations in the medial frontal gray matter and left frontal white matter. Metabolite levels were correlated with Glasgow Coma Scale (GCS) scores and neurobehavioral functioning. There was a trend for lower NAA concentrations in the medial frontal gray matter for the TBI group. Late NAA and Cr levels in the medial frontal gray matter and NAA levels in the left frontal white matter were strongly positively correlated with initial GCS score. Metabolite levels were correlated with some neurobehavioral measures differentially for children with TBI or OI. Some neurometabolite levels differed between the TBI and OI groups more than 1 year post-injury and were related to injury severity, as well as some neurobehavioral outcomes following TBI during early childhood.