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The ubiquity of aerosols in the atmosphereespecially the tropospheremakes them a vital component of climate models as well as air pollutants through the impact on human health. It has become clear that organic aerosols (OAs) are an important fraction of the aerosol mass and thus need to be considered explicitly in models and regulations. Determining the origins of OAs from primary sources (e.g., biomass burning, urban emissions) is difficult enough, but the atmospheric organic carbon budget is heavily influenced by the formation of secondary OAs from gas-phase precursors. In this Feature, de Gouw and Jimenez briefly summarize what observations and models seem to be saying, and highlight what more needs to be elucidated for improved modeling accuracy.