The DEVOTE research project aimed at the novel installation of an aerosol research airborne platform comprised of two aircraft. The first functions as an airborne suborbital simulator for the next generation of Earth-orbiting satellites devoted to climate studies and includes the NASA GISS Research Scanning Polarimeter (RSP) and the NASA Langley High Spectral Resolution Lidar (HSRL); the second provides a complete suite of in situ instruments (LARGE) and a hygrometer (DLH) to validate the remote measurements. With both aircraft based at the NASA Langley Research Center, the platform can be deployed on a very short notice to survey aerosol events of interest. We present an overview of the recently completed mission that exceeded the expected results. Eleven research flights were successfully completed over a vast area spanning the Eastern and Southern United States, providing coincident measurements of several aerosol conditions, ranging from urban pollution to agricultural fires to marine scenarios. Selected flight legs were also coordinated with A-Train overpasses and with seven different AERONET stations on the ground. The archived dataset, available to the public starting May 2012, contains therefore a unique merge of state-of-the-art aerosol measurements including size, extinction, humidification and vertical distribution together with a characterization of the polarization signatures. The latter stems from the first simultaneous deployment of the RSP and the UMBC Polarization Imaging Nephelometer that was developed as part of the project. The DEVOTE proposal was awarded by the NASA HOPE-TO program to train early-career atmospheric scientists to the management of a full life-cycle scientific mission.