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PM10 was collected during an EMEP winter campaign of 2017-2018 in two urban background sites in Barcelona (BCN) and Granada (GRA), two Mediterranean cities in the coast and inland, respectively. The concentrations of PM10, organic carbon (OC), elemental carbon (EC), and organic molecular tracer compounds such as hopanes, anhydro-saccharides, polycyclic aromatic hydrocarbon, and several biogenic and anthropogenic markers of secondary organic aerosols (SOA) were two times higher in GRA compared to BCN and related to the atmospheric mixing heights in the areas. Multivariate curve resolution (MCR-ALS) source apportionment analysis identified primary emissions sources (traffic + biomass burning) that were responsible for the 50% and 20% of the organic aerosol contributions in Granada and Barcelona, respectively. The contribution of biomass burning was higher in the holidays than in the working days in GRA while all primary combustion emissions decreased in holidays in BCN. The MCR-ALS identified that oxidative species and SOA formation processes contributed to 40% and 80% in Granada and Barcelona, respectively. Aged SOA was dominant in Granada and Barcelona under stagnant atmospheric conditions and in presence of air pollution. On the other hand, fresh SOA contributions from α-pinene oxidation (cis-pinonic acid) were three times higher in Barcelona than Granada and could be related to new particle formation, essentially due to overall cleaner air conditions and elevated air temperatures. ; Financial support for this study was provided by the Cooperative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollution in Europe (EMEP) and the European Union's Horizon 2020 research project ACTRIS2 (654109) and supported by research projects from the Plan Nacional de IyD of the Spanish Ministry of Science and Innovation INTEMPOL (PGC2018-102288-B-I00), HOUSE (CGL2016-78594-R), and BioCloud (RTI2018.101154.A.I00). IDAEA-CSIC is a Severo Ochoa Centre of Research Excellence (Spanish Ministry of Science and Innovation, CEX2018-000794-S). ; Peer reviewed