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Although social disorganization theory and institutional anomie theory have received considerable empirical support in the literature, both theories also leave a substantial amount of variation in macro-level crime unexplained. Based on the theoretical integration approach in criminology, this study develops a more comprehensive framework to predict neighborhood crime by simultaneously testing neighborhood-level social disorganization measures and county-level institutional anomie measures. More specifically, it empirically tests an integrated theory of macro-level crime utilizing National Neighborhood Crime Study data from 9,593 neighborhoods nested within 64 urban counties in the United States using multilevel and geospatial analysis methods. Cross-level interaction terms are used with multilevel overdispersed Poisson models to test the moderating effects of eight different measures county-level economic dominance and the strength of commitment to five noneconomic institutions, on the relationship between social disorganization predictors and neighborhood crime rates. The findings support the effects of three structural social disorganization measures and county-level economic inequality measures on neighborhood crime rates, yield some support for the moderation hypotheses, and can be applied to develop targeted intervention programs for law enforcement and criminal justice agencies.