The Aerosols99 cruise crossed the Atlantic Ocean from Norfolk, Virginia, to Cape Town, South Africa, between January 14 and February 8, 1999. The goals of the cruise were to determine the chemical, physical, and optical properties of the marine boundary layer (MBL) aerosol, the vertical distribution of aerosols and ozone, the column-integrated aerosol optical depth, and the ozone, CO, and peroxy radical chemistry in the MBL. Sampling strategies were optimized to obtain data sets to evaluate satellite-derived ocean color (Sea-viewing Wide Field-of-view Sensor), aerosol optical depth (advanced very high resolution radiometer) and total column ozone (Total Ozone Mapping Spectrometer). The cruise track crossed through seven different meteorological/oceanographic regimes ranging from background marine air masses in the Northern and Southern Hemispheres to air masses containing mineral dust and the products of biomass burning. This overview discusses the seven regimes encountered enroute and the chemical and physical properties of the MBL aerosol in each regime.