Nuclear accidents and decommissioning in the nuclear industry would release a large number of radioactive aerosols which endangers the natural environment and the health of workers. Therefore, there is an urgent need for environment-friendly aerosol suppressants to control and handle environmental pollution problems caused by radioactive aerosols. In this paper, sodium alginate (SA), a type of polyphenol material (TP), and alkyl glycosides (APGs) were selected as the components of the compound aerosol suppressant and the optimal proportion was generated via the method of D-optimal mixture design. Furthermore, the cesium aerosol sedimentation effect of the optimized compound aerosol suppressants was evaluated via sedimentation efficiency, the change in particle concentration cumulative concentration fraction of the cesium aerosol sedimentation process. The results showed that the aerosol sedimentation efficiency was 99.82% which was much higher than nature settlement, 18.6% and water spraying sedimentation, 43.3%. Moreover, after spraying the compound suppressant, it displayed a good effect on settling the cesium aerosol particles with a diameter of less than 1 µm, as the concentration of particles was reduced from 55.49% to 44.53%. Finally, the sedimentation mechanism of the compound aerosol suppressant and cesium aerosol particles, such as the coagulation effect, was analyzed using the particle size distribution.