We offer an overview of the COVID-19 -driven air quality changes across 11 metropolises in Spain with the focus on lessons learned on how continuing abating pollution. Traffic flow decreased by up to 80% during the lockdown and remained relatively low during the full relaxation (June and July). After the lockdown a significant shift from public transport to private vehicles (+21% in Barcelona) persisted due to the pervasive fear that using public transport might increase the risk of SARS-CoV-2 infection, which need to be reverted as soon as possible. NO
2
levels fell below 50% of the WHO annual air quality guidelines (WHOAQGs), but those of PM
2.5
were reduced less than expected due to the lower contributions from traffic, increased contributions from agricultural and domestic biomass burning, or meteorological conditions favoring high secondary aerosol formation yields. Even during the lockdown, the annual PM
2.5
WHOAQG was exceeded in cities within the NE and E regions with high NH
3
emissions from farming and agriculture. Decreases in PM
10
levels were greater than in PM
2.5
due to reduced emissions from road dust, vehicle wear, and construction/demolition. Averaged O
3
daily maximum 8-h (8hDM) experienced a generalized decrease in the rural receptor sites in the relaxation (June–July) with −20% reduced mobility. For urban areas O
3
8hDM responses were heterogeneous, with increases or decreases depending on the period and location. Thus, after canceling out the effect of meteorology, 5 out of 11 cities experienced O
3
decreases during the lockdown, while the remaining 6 either did not experience relevant reductions or increased. During the relaxation period and coinciding with the growing O
3
season (June–July), most cities experienced decreases. However, the O
3
WHOAQG was still exceeded during the lockdown and full relaxation periods in several cities. For secondary pollutants, such as O
3
and PM
2.5
, further chemical and dispersion modeling along with source apportionment techniques to identify major precursor reduction targets are required to evaluate their abatement potential.
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