In the foreseen decommissioning and debris removal plans of the damaged Fukushima Daiichi reactors, the fuel debris will be broken into small pieces using laser or mechanical cutting techniques prior to removing them from the reactor buildings. Regardless of the technique to be employed, submicron radioactive aerosol particles will be generated and dispersed in the gas space of primary containment vessel during cutting operations. The water spray system has been proven to be an applicable method in removing aerosol particles. However, it cannot remove Greenfield-gap aerosol particles (with diameters between 0.1–1 μm) so effectively. To solve this problem, a new agglomeration method by addition of water mist before spray injection was developed. With preexisting water mist, aerosol particles were expected to aggregate with water mist and form larger-sized agglomerated aerosol-mist particles, which increased the effect of inertial impaction mechanism leading to higher scavenging efficiency. The new method has been verified to be capable of improving the spray scavenging efficiency for the Greenfield gap particles by conducting aerosol scavenging experiments without and with mist in the newly built UTARTS facility in the University of Tokyo. The experiment results showed that the aerosol removal rate increased along with the increasing of mist concentration level. To verify the new agglomeration method in different experiment facilities and to investigate the effects of vessel’s size scale on aerosol collection efficiency, similar experiments were repeated in the TOSQAN facility of IRSN, France. Though the cylindrical vessel in two facilities have same internal diameter, the vessel’s height of TOSQAN facility is 4.8 m, which is larger than the one in the UTARTS facility (2.5 m). The experiment results in TOSQAN facility also showed that water mist has potential to improve aerosol spray scavenging efficiency. The corresponding numerical simulations about aerosol removal by spray droplets without mist in both UTARTS and TOSQAN facilities were conducted to better understand the aerosol removal process, including time evolution of aerosol mass fraction and flow field of the gas phase.