Aedes albopictus is the primary vector of dengue fever and dengue hemorrhagic fever in China. Although there are previous studies on the application of adulticides to control this species, the application methods have either been back-pack or vehicle-mounted systems. However, many sites are too large to be effectively treated with back-pack sprayers, and the lack of roads restricts the use of vehicle-mounted sprayers. This paper provides the first study of using unmanned aerial vehicles to conduct cold mist sprays on Ae. albopictus habitats. A spray containing 4% permethrin and 1% tetramethylfluthrin was applied at an effective application rate of 9.0 mg/m². This method reduced Ae. albopictus populations by more than 90%. The results indicate this novel spray system is a powerful method to achieve a rapid decline of mosquito population in Ae. albopictus habitats in China.