The decommissioning of nuclear facilities and nuclear accidents may release a various amount of radioactive aerosols, which could pose a serious threat to the natural environment and human health. Therefore, there is a need to develop an eco-friendly aerosol suppressant to control the radioactive aerosol. In this paper, carboxymethyl cellulose (CMC), polyvinyl alcohol (PVA), rhamnolipid and sophorajaponica glycolipid were selected as the raw material, and the aerosol suppressant was prepared by solution polymerization. The sample was characterized by FTIR, TGA, viscosity, surface tension and contact angle analysis. The results indicated that the grafted reaction was successful. Rhamnolipid and sophorajaponica glycolipid effectively reduced the surface tension of the copolymer solution to 27.7 mN/m, and the contact angle between the polymer solution and experimental dust was decreased to 27.36°. The aerosol sedimentation experiment showed that the suppressant had a significant effect on aerosol. The sedimentation efficiency of concrete aerosols was 87.7%, and the sedimentation efficiency of radioactive aerosols reached 90.8%. It provided an eco-friendly and effective method to quickly and easily control and remove high-concentration radioactive aerosol.