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Segregation is argued to weaken social controls and undermine a community’s regulatory capacity through mechanisms associated with social inequality and social isolation. However, empirical support for this relationship is far from conclusive. To date, most segregation-crime studies concentrate on segregation patterns at the city level using indices that ignore the spatiality of segregation. In this paper we employ highly spatialized measures of local residential segregation to unpack the relationship between segregation, inequality and crime across 297 neighborhoods located in two Australian cities with differing immigration histories and ethnic compositions. Drawing on survey, census and crime data, we additionally consider the role collective efficacy plays in mediating or moderating the association between segregation, inequality and crime.