This review focuses on critical issues in ocean–atmosphere exchange that will be addressed by new research strategies developed by the international Surface Ocean–Lower Atmosphere Study (SOLAS) research community. Eastern boundary upwelling systems are important sites for CO2 and trace gas emission to the atmosphere, and the proposed research will examine how heterotrophic processes in the underlying oxygen-deficient waters interact with the climate system. The second regional research focus will examine the role of sea-ice biogeochemistry and its interaction with atmospheric chemistry. Marine aerosols are the focus of a research theme directed at understanding the processes that determine their abundance, chemistry and radiative properties. A further area of aerosol-related research examines atmospheric nutrient deposition in the surface ocean, and how differences in origin, atmospheric processing and composition influence surface ocean biogeochemistry. Ship emissions are an increasing source of aerosols, nutrients and toxins to the atmosphere and ocean surface, and an emerging area of research will examine their effect on ocean biogeochemistry and atmospheric chemistry. The primary role of SOLAS is to coordinate coupled multi-disciplinary research within research strategies that address these issues, to achieve robust representation of critical ocean–atmosphere exchange processes in Earth System models.