The nexus between substance use and aggressive crime involves a complex interrelationship among mediating individual and community-level variables. Using multilevel logistic regression models, we investigate how community-level concentration of poverty variables mediate the predictive relationships among individual level social attachment variables and substance use on aggressive crime in a large national sample of male arrestees (N = 20,602) drawn from 24 U.S. urban areas. The findings support our hypothesis that individual social attachments to marriage and the labor force (education and employment) are the principal individual-level pathway mediating the substance abuse/aggression nexus. In the random intercept model, 3.17% of the variation not explained by the individual-level predictor variables is attributable to community-level variation in urban area female-headed households and households receiving welfare. This confirms our hypothesis that social structural conditions of an urban environment differentially expose persons to conditions that predict being arrested for an aggressive crime. Our findings tend to counter the cultural theorists who argue for an indigenous culture of violence in inner-city ghettos and barrios.