The comprehensive investigation of polar ozone photochemistry and dynamics has required data obtained from as full a complement of available platforms as possible (ground-based, balloon, aircraft, and satellites). Perhaps the most detailed process studies have been conducted using measurements from aircraft, taking advantage of their targeting capabilities coupled with the potential for enabling measurements at high spatial and temporal resolution. The US National Aeronautics and Space Administration (NASA) conducted the first airborne science investigation of polar ozone in an effort to establish the causes of the recurring seasonal depletion of the Earth's stratospheric ozone layer over Antarctica that was identified in the mid-1980s. Subsequent airborne studies in the polar regions of both hemispheres benefitted from extensive successful collaborations among international scientists and the integration of the aircraft measurements with those obtained using ground-based, balloon-borne, and satellite instruments. This article provides an historical perspective of NASA's utilization of its airborne assets to advance our understanding of the chemical and physical processes that control the abundance of stratospheric ozone in both the Antarctic and Arctic.