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Background: Glyoxal has been implicated as a significant contributor to the formation of secondary organic aerosols, which play a key role in our ability to estimate the impact of aerosols on climate. Elevated concentrations of glyoxal over remote ocean waters suggests that there is an additional source, distinct from urban and forest environments, which has yet to be identified. Herein, we demonstrate that the ocean can serve as an appreciable source of glyoxal in the atmosphere due to microbiological activity. Methods and Results: Based on mass spectrometric analyses of nascent sea spray aerosols and the sea surface microlayer (SSML) of naturally occurring algal blooms, we provide evidence that during the algae death phase phospholipids become enriched in the SSML and undergo autoxidation thereby generating glyoxal as a degradation product. Conclusions: We propose that the death phase of an algal bloom could serve as an important and currently missing source of glyoxal in the atmosphere.