Plasma technology has been employed for the removal of gaseous elemental mercury (Hg0) from simulated flue gases without pre-existing airborne particles. This study developed a double dielectric barrier discharge (DDBD) treatment system, in which two coaxial electrodes were covered by quartz dielectrics, for removing mercury with the presence of aerosol particles. The increase in pre-existing aerosol surface concentration can improve Hg0 removal efficiency up to 160% in the DDBD device. Inorganic aerosol particles (sodium chloride) perform better than organic ones (sucrose) in improving Hg0 removal efficiency. These aerosol particles can be collected in the DDBD system. For sodium chloride particles, a collection efficiency of more than 90% was observed in the tested diameter range of 10–100 nm. The improvement in Hg0 removal with the presence of particles is possibly due to that (i) aerosol particles provide additional surface for surface-induced Hg0 oxidations, (ii) reactive species (such as Cl) generated by plasma etching particle surface rapidly react with Hg0, and (iii) charged particles can in-flight adsorb mercury species.