Traumatic brain injury (TBI) is highly prevalent in adults. TBI-related functional brain alterations have been linked with common post-TBI neurobehavioral sequelae, with unknown neural substrates. This study examined the systems-level functional brain alterations in white matter (WM) and gray matter (GM) for visual sustained-attention processing, and their interactions and contributions to post-TBI attention deficits. Task-based functional MRI data were collected from 42 adults with TBI and 43 group-matched normal controls (NCs), and analyzed using the graph theoretic technique. Global and nodal topological properties were calculated and compared between the two groups. Correlation analyses were conducted between the neuroimaging measures that showed significant between-group differences and the behavioral symptom measures in attention domain in the groups of TBI and NCs, respectively. Significantly altered nodal efficiencies and/or degrees in several WM and GM nodes were reported in the TBI group, including the posterior corona radiata (PCR), posterior thalamic radiation (PTR), postcentral gyrus (PoG), and superior temporal sulcus (STS). Subjects with TBI also demonstrated abnormal systems-level functional synchronization between the PTR and STS in the right hemisphere, hypo-interaction between the PCR and PoG in the left hemisphere, as well as the involvement of systems-level functional aberrances in the PCR in TBI-related behavioral impairments in the attention domain. The findings of the current study suggest that TBI-related systems-level functional alterations associated with these two major-association WM tracts, and their anatomically connected GM regions may play critical role in TBI-related behavioral deficits in attention domains.