There is mounting concern for the health of urban populations as cities expand at an unprecedented rate. Urban green spaces provide settings for a remarkable range of physical and mental health benefits, and pioneering health policy is recognizing nature as a cost-effective tool for planning healthy cities. Despite this, limited information on how specific elements of nature deliver health outcomes restricts its use for enhancing population health. We articulate a framework for identifying direct and indirect causal pathways through which nature delivers health benefits, and highlight current evidence. We see a need for a bold new research agenda founded on testing causality that transcends disciplinary boundaries between ecology and health. This will lead to cost-effective and tailored solutions that could enhance population health and reduce health inequalities.