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Adopting electric end-use technologies instead of fossil-fueled alternatives, known as electrification, is an important economy-wide decarbonization strategy that also reduces criteria pollutant emissions and improves air quality. In this study, we evaluate CO2 and air quality co-benefits of electrification scenarios by linking a detailed energy systems model and a full-form photochemical air quality model in the United States. We find that electrification can substantially lower CO2 and improve air quality and that decarbonization policy can amplify these trends, which yield immediate and localized benefits. In particular, transport electrification can improve ozone and fine particulate matter (PM2.5), though the magnitude of changes varies regionally. However, growing activity from non-energy-related PM2.5 sources—such as fugitive dust and agricultural emissions—can offset electrification benefits, suggesting that additional measures beyond CO2 policy and electrification are needed to meet air quality goals. We illustrate how commonly used marginal emissions approaches systematically underestimate reductions from electrification. Electrification is a decarbonization strategy that has the potential to reduce pollutant emissions and improve air quality. Here the authors evaluate CO2 and air quality co-benefits of electrification scenarios in the United States and find that electrification can substantially lower CO2 and improve ozone and fine particulate matter regionally. [ABSTRACT FROM AUTHOR]