Neighborhood-level social determinants are increasingly recognized as factors shaping mental health in adults. Data-driven informatics methods and geographic information systems (GIS) offer innovative approaches for quantifying neighborhood attributes and studying their influence on mental health. Guided by a modification of Andersen's Behavioral Model of Health Service Use framework, this cross-sectional study examined associations of neighborhood resource groups with psychological distress and depressive symptoms in 1,528 U.S. Veterans. Data came from the Veteran Affairs (VA) Health Services Research and Development Proactive Mental Health trial and publicly available sources. Hierarchical clustering based on the proportions of neighborhood resources within walkable distance was used to identify neighborhood resource groups and generalized estimating equations analyzed the association of identified neighborhood resource groups with mental health outcomes. Few resources were found in walkable areas except alcohol and/or tobacco outlets. In clustering analysis, four meaningful neighborhood groups were identified characterized by alcohol and tobacco outlets. Living in an alcohol-permissive and tobacco-restrictive neighborhood was associated with increased psychological distress but not depressive symptoms. Living in urban or rural areas and access to VA care facilities were not associated with either outcome. These findings can be used in developing community-based mental health-promoting interventions and public health policies such as zoning policies to regulate alcohol outlets in neighborhoods. Augmenting community-based services with Veteran-specialized services in neighborhoods where Veterans live provides opportunities for improving their mental health.