Few challenges pose a greater threat to a healthy planet and people than air pollution and climate change. Over the past three decades, research has demonstrated that integrated solutions to air pollution and climate change can yield co-benefits that support cost-effective, coherent policies. However, research on co-benefits has yet to generate policy responses consistent with this promise. This paper argues that realizing this potential requires more rigorous research on how governance affects the opportunities and incentives to align the interests of government agencies, scientists, and other stakeholders at multiple levels. The article proposes a “One Atmosphere approach” consisting of three building blocks to strengthen that alignment: (1) continually incorporating and strategically timing the introduction of integrated visions; (2) reforming governance arrangements to encourage interagency collaboration and multi-stakeholder cooperation; and (3) supporting integrated visions and institutional cooperation with standardized metrics and assessment methods. This article is also the introduction to the Special Issue ‘One Atmosphere: Integrating Air Pollution and Climate Policy and Governance’, aimed at fostering the multidisciplinary dialogue needed for more integrated air pollution and climate change policies.