In recent decades, better data and methods have become available for understanding the complex functioning of cities and their impacts on sustainability. This review synthesizes the recent developments in concepts and methods being used to measure the impacts of cities on environmental sustainability. It differentiates between a dominant trend in research literature that concentrates on the accounting and allocation of greenhouse gas emissions and energy use to cities and a reemergence of studies that focus on the direct and indirect material and resource flows in cities. The methodological approaches reviewed may consider cities as either producers or consumers, and all recognize that urban environmental impacts can be local, regional, or global. As well as giving an overview of the methodological debates, we examine the implications of the different approaches for policy and the challenges these approaches face in their application in the field.