ABSTRACT: Antisocial behavior (AB), including violence, criminality, and substance abuse, is often linked to deficits in emotion processing, reward-related learning, and inhibitory control, as well as their associated neural networks. To better understand these deficits, the structural connections between brain regions implicated in AB can be examined using diffusion tensor imaging (DTI), which assesses white matter microstructure. Prior studies have identified differences in white matter microstructure of the uncinate fasciculus (UF), primarily within offender samples. However, few studies have looked beyond the UF or determined whether these relationships are present dimensionally across the range of AB and callous-unemotional (CU) traits. In the current study, we examined associations between AB and white matter microstructure from major fiber tracts, including the UF. Further, we explored whether these associations were specific to individuals high on CU traits. Within a relatively large community sample of young adult men from low-income, urban families (N?=?178), we found no direct relations between dimensional, self-report measures of either AB or CU traits and white matter microstructure. However, we found significant associations between AB and white matter microstructure of several tracts only for those with high co-occurring levels of CU traits. In general, these associations did not differ according to race, socioeconomic status, or comorbid psychiatric symptoms. The current results suggest a unique neural profile of severe AB in combination with CU traits, characterized by widespread differences in white matter microstructure, which differs from either AB or CU traits in isolation and is not specific to hypothesized tracts (i.e., the UF).