One of the biggest challenges facing researchers trying to empirically test structural or institutional anomie theories is the operationalization of the key concept of anomie. This challenge is heightened by the data constraints involved in cross-national research. As a result, researchers have been forced to rely on surrogate or proxy measures of anomie and indirect tests of the theories. The purpose of this study is to examine an innovative and more theoretically sound measure of anomie and to test its ability to make cross-national predictions of serious crime. Our results are supportive of the efficacy of this construct to explain cross-national variations in crime rates. Nations with the highest rates of structural anomie also have the highest predicted rates of homicide.