It is well established that in Europe, high O 3 concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to O 3 formation within each country relative to the imported (regional and hemispheric) O 3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the O 3 target value set by the European air quality directive. O 3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O 3 and precursors from neighbouring regions, O 3 regional and hemispheric transport and stratospheric O 3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O 3 events in Spain relative to the contribution of imported (regional and hemispheric) O 3 . We also assess the potential of our source apportionment method to improve O 3 modelling. Our study applies and thoroughly evaluates a countrywide O 3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4 km 2 ) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O 3 and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical pro-cesses (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NO x local sources to high O 3 concentrations compared with the contribution of imported O 3 . We show, for the first time, that imported O 3 is the largest input to the ground-level O 3 concentration in the IP, accounting for 46 %-68 % of the daily mean O 3 concentration during exceedances of the European target value. The hourly imported O 3 increases during typical northwestern advections (70 %-90 %, 60-80 µg m −3 ), and decreases during typical stagnant conditions (30 %-40 %, 30-60 µg m −3 ) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the O 3 peaks in areas downwind of the main urban and industrial regions (up to 40 % in hourly peaks). We also show that ground-level O 3 concentrations are strongly affected by vertical mixing of O 3 -rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported O 3 at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high O 3 concentrations for local O 3 management, and show O 3 source apportionment to be an ess...