Desert dust outbreaks may affect air quality. This study estimates the importance of African dust contribution to the PM10 and PM2.5 concentrations observed in rural regional background sites in Portugal. Desert dust contribution is evaluated by two different approaches: A measurement-approach methodology based on the monthly moving 40th percentile, and a model-approach methodology based on WRF-CHIMERE simulations, whose performance is also assessed within this work. Several desert dust episodes affected atmospheric aerosols in the planetary boundary layer over Portugal during 2016. Their intensity was variable, with at least two events (21–22 February and 27–28 October) contributing to exceedances to the PM10 daily limit value defined in the European Air Quality Directive. African dust contributions obtained for the year 2016 with the measurement-approach methodology are higher than the ones simulated by WRF-CHIMERE. Contributions to PM10 and to PM2.5 concentrations range from 0 to 90 µg m−3 and from 0 to 30 µg m−3, respectively, in most of the regions and days. Caution must be employed when using measurement-approach methodologies to quantify dust contributions to PM levels when forest fires occur simultaneously with the long-range transport of desert dust, as happened in August 2016.