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This manuscript reported data for total suspended particulate matter (TSPM), particle-bound mercury (PBM), and total gaseous mercury (TGM) in Almadenejos, a rural zone of ancient Hg mining and metallurgical works. Concentrations of TSPM characterize the study site as being a rural area, with levels below 40 μg m -3 during most of the year and sporadic events involving dust intrusions from Africa. Mercury speciation of PM and nearby soils, which contain both cinnabar and organic Hg, confirms that the PM comes from local soil emissions involving the soils polluted by ancient metallurgical works. Conversely, PBM and TGM levels (average 1.8 ng m -3 and 88 ng m -3 , respectively) define Almadenejos as a contaminated site similar to urban areas. A multiple linear regression analysis showed that evapotranspiration is the micrometeorological parameter that best explains the TSPM and PBM data, with the creation of a diurnal mixing layer being the main process involved in Hg emissions in the solid and gaseous states. Based on these findings, a micrometeorological-based model has been developed to acquire a complete set of daily PBM data and these were used to obtain dry deposition rates (317 μg m -2  year -1 ), which were seasonally distributed as 40% in summer, 33% in autumn, 16% in spring, and 11% in winter. In addition, an estimation of PBM emissions showed that 335 g year -1 can be suspended in the Almadenejos environment. A large proportion of this PBM should be removed from the atmosphere through dry deposition in a continuous Hg exchange at the soil-atmosphere interface. Mercury fractionation (cinnabar and organic Hg) can increase the risk to the human population and nearby ecosystems of Almadenejos.