The water–energy–food nexus is being promoted as a conceptual tool for achieving sustainable development. Frameworks for implementing nexus thinking, however, have failed to explicitly or adequately incorporate sustainable livelihoods perspectives. This is counterintuitive given that livelihoods are key to achieving sustainable development. In this paper we present a critical review of nexus approaches and identify potential linkages with sustainable livelihoods theory and practice, to deepen our understanding of the interrelated dynamics between human populations and the natural environment. Building upon this review, we explore the concept of ‘environmental livelihood security’ – which encompasses a balance between natural resource supply and human demand on the environment to promote sustainability – and develop an integrated nexus-livelihoods framework for examining the environmental livelihood security of a system. The outcome is an integrated framework with the capacity to measure and monitor environmental livelihood security of whole systems by accounting for the water, energy and food requisites for livelihoods at multiple spatial scales and institutional levels. We anticipate this holistic approach will not only provide a significant contribution to achieving national and regional sustainable development targets, but will also be effective for promoting equity amongst individuals and communities in local and global development agendas.