The immense impacts of coal-fired power plant plumes on the atmospheric environment have caused great concern linked to climate and health issues. However, studies on the field observations of aerial plumes are relatively limited, mainly due to the lack of suitable plume observation tools and techniques. In this study, we use a multicopter unmanned aerial vehicle (UAV) sounding technique to study the influences of the aerial plumes of the world's fourth-largest coal-fired power plant on the atmospheric physical/chemical conditions and air quality. A set of species, including 106 volatile organic compounds (VOCs), CO, CO2, CH4, PM2.5, and O3, and meteorological variables of temperature (T), specific humidity (SH), and wind data, are collected by the UAV sounding technique. The results reveal that the large-scale plumes of the coal-fired power plant cause local temperature inversion and humidity changes, and even affect the dispersion of pollutants below. The chemical compositions of coal-fired power plant plumes are significantly different from those of another ubiquitous vehicular source. High fractions of ethane, ethene, and benzene and low fractions of n-butane and isopentane found in plumes could serve as the key features to help distinguish the influences of coal-fired power plant plumes from other pollution sources in a particular area. By taking the ratios of pollutants (e.g., PM2.5, CO, CH4, and VOCs) to CO2 in plumes and the CO2 emission amounts of the power plant into calculation, we enable the easy quantification of the specific pollutant emissions released from power plant plumes to the atmosphere. In summary, observation by using drone soundings dissecting the aerial plumes provides a new methodology that allows aerial plumes to be readily detected and characterized. Furthermore, the influences of the plumes on the atmospheric physical/chemical conditions and air quality can be assessed rather straightforwardly, which was not easily achievable in the past.