This Special Issue provides the first literature collection focused on the development and implementation of unmanned aircraft systems (UAS) and their integration with sensors for atmospheric measurements on Earth. The research covered in the Special Issue combines chemical, physical, and meteorological measurements performed in field campaigns as well as conceptual and laboratory work. Useful examples for the development of platforms and autonomous systems for environmental studies are provided, which demonstrate how careful the operation of sensors aboard UAS must be to gather information for remote sensing in the atmosphere. The work serves as a key collection of articles to introduce the topic to new researchers interested in the field, guide future studies, and motivate measurements to improve our understanding of Earth’s complex atmosphere. The next section summarizes the key information of individual contributions