The Flight Research Laboratory of the National Research Council of Canada has an active program of airborne atmospheric research that has been realized primarily in collaboration with other Canadian, as well as American, agencies. The current focus is on global change science, aircraft icing and airborne remote sensing system development. Over the past 50 years, research has been conducted on a diverse array of science and technology issues, driven by contemporary aerospace concerns and, more generally, national and societal needs of the day. The Laboratory's initial efforts in airborne atmospheric science started in 1953, and included work in helicopter icing, work in aircraft structural integrity under turbulent conditions, as well as studies to characterize atmospheric turbulence in general. Presently, projects in the realm of airborne atmospheric science have been organized around the Twin Otter and the Convair 580 aircraft. In recent years, these aircraft have been developed to support research efforts in aircraft icing (Convair 580), air quality and global change science (Twin Otter), as well as remote sensing of the atmosphere and the Earth (both the Convair 580 and the Twin Otter). A particular strength is the precise measurement of atmospheric motion - which, in turn, permits a well-regarded capability in airborne flux measurement (the measurement of the total vertical flow of a quantity of interest, i.e., water vapour or heat). This paper includes brief summaries of the flight envelopes and the instrumentation on-board the Twin Otter and Convair 580 when configured for atmospheric research. The variety and application of the data collected by these aircraft are demonstrated with examples from several recent experiments.