Brain structure is often studied as a marker of youth psychopathology by examining associations between volume or thickness of individual regions and specific diagnoses. However, these univariate approaches do not address whether the effect of a particular region may depend on the structure of other regions. Here, we identified subgroups of individuals with distinct profiles of brain structure and examined how these profiles were associated with concurrent and future youth psychopathology. We used latent profile analysis to identify distinct neuroanatomical profiles of subcortical region volume and orbitofrontal cortical thickness in the ABCD study (N = 9376, mean age = 9.91, SD = 0.62). We identified a five-profile solution consisting of a reduced subcortical volume profile, a reduced orbitofrontal thickness profile, a reduced limbic and elevated striatal volume profile, an elevated orbitofrontal thickness and reduced striatal volume profile, and an elevated orbitofrontal thickness and subcortical volume profile. While controlling for age, sex, and intracranial volume, profiles exhibited differences in concurrent psychopathology measured dimensionally and categorically and in psychopathology at 1-year follow-up measured dimensionally. Results show that profiles of brain structure have incremental validity for associations with youth psychopathology beyond intracranial volume.