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The sea surface microlayer (SML) is the boundary interface between the atmosphere and ocean, covering about 70% of the Earth’s surface. With an operationally defined thickness between 1 and 1000 μm, the SML has physicochemical and biological properties that are measurably distinct from underlying waters. Recent studies now indicate that the SML covers the ocean to a significant extent, and evidence shows that it is an aggregate-enriched biofilm environment with distinct microbial communities. Because of its unique position at the air-sea interface, the SML is central to a range of global biogeochemical and climate-related processes. The redeveloped SML paradigm pushes the SML into a new and wider context that is relevant to many ocean and climate sciences.