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The Italian Po Valley is one of the most polluted regions in Europe. During winter, meteorological conditions favor long and dense fogs, which strongly affect visibility and human health. In spring, the frequency of nighttime fogs reduces while daytime new particle formation events become more common. This transition is likely caused by a reduction in particulate matter (PM2.5), leading to a decrease in the relevant condensation sink. The physics and chemistry of fog and aerosol have been studied at the San Pietro Capofiume site since the 1980s, but the detailed processes driving the observed trends are not fully understood. Hence, during winter and spring 2021/22, the Fog and Aerosol Interaction Research Italy (FAIRARI) campaign was carried out, using a wide spectrum of approaches, including in situ measurements, outdoor chamber experiments, and remote sensing. Atmospheric constituents and their properties were measured ranging from gas molecules and molecular clusters to fog droplets. One unique aspect of this study is the direct measurement of the aerosol composition inside and outside of fog, showing a slightly greater dominance of organic compounds in the interstitial compared to the droplet phase. Satellite observations of fog provided a spatial context and agreed well with in situ measurements of droplet size. They were complemented with in situ chamber experiments, providing insights into oxidative processes and revealing a large secondary organic aerosol-forming potential of ambient air upon chemical aging. The oxidative potential of aerosol and fog water inferred the impact of aerosol–fog interactions on particle toxicity. SIGNIFICANCE STATEMENT: Aerosol and fog influence our climate and can have adverse effects on human health and visibility. Through anthropogenic emissions, such as from industry or transport, humans can influence the physical and chemical properties of fog and aerosol. The FAIRARI campaign investigated the formation of aerosols and aerosol–fog interactions in the Italian Po Valley, one of the most polluted regions in Europe. State-of-the-art experimental methods revealed the details of aerosols and fogs from the molecular level to the droplet scale. We observed a clear transition from winter to spring, with fog-dominated periods followed by an intensified secondary aerosol formation period. Organic and nitrate compounds dominated the composition of aerosol and fog residuals. The results will contribute to various aerosol–fog interaction modeling activities. [ABSTRACT FROM AUTHOR]