This paper describes a unique validation data set acquired from a marine intensive observing period (IOP) conducted on board the NOAA Ship Ronald H. Brown (RHB) during the 2004 Aerosol and Ocean Science Expedition (AEROSE) in the tropical North Atlantic Ocean from 29 February to 26 March 2004. The radiometric and in situ data complement includes marine observations of the Saharan air layer (SAL), including two significant Saharan dust outbreaks over the Atlantic Ocean. Because the impact of tropospheric dust aerosols on satellite infrared (IR) radiometric observations has not yet been fully characterized, the AEROSE data are particularly valuable for IR sensor validation. Shipboard radiometric data germane to satellite validation include observations from a Marine Atmospheric Emitted Radiance Interferometer (M-AERI), a Calibrated Infrared In situ Measurement System (CIRIMS), and Microtops handheld sunphotometers. Among other things, these data provide, for the first time, coincident IR spectra of the dry, dusty SAL from both the uplooking M-AERI and the downlooking Atmospheric Infrared Sounder (AIRS) on board the Aqua satellite. In situ data collected throughout the cruise include Vaisala RS80/90 radiosondes, launched $simeq$3-hourly to include Aqua overpass times. The Aqua matchup profiles provide data for validation of AIRS in the presence of high dust loading, along with temperature and water vapor profile retrievals of the SAL. The frequency of sonde launches also enables validation of coincident uplooking M-AERI boundary layer profile retrievals. Preliminary analyses of the AEROSE data are presented here. Focused AEROSE validation studies are the subjects of separate papers.