In situ and laser remote measurements of gases and aerosols were made with airborne instrumentation to investigate the sources and sinks of tropospheric gases and aerosols over the tropical South Atlantic during the NASA Global Tropospheric Experiment (GTE)/Transport and Atmospheric Chemistry Near the Equator-Atlantic (TRACE A) field experiment conducted in September–October 1992. Gases from extensive fires in Brazil were transported by convective storms into the upper troposphere where tropospheric ozone (O3) was photochemically produced and advected eastward over the South Atlantic. In central Africa, the fires were widespread, and in the absence of deep convection, the fire plumes were advected at low altitudes (below ∼6 km) over the Atlantic. There was a positive correlation between O3 and aerosols found in the plumes that were not involved in convection. High O3 (>75 parts per billion by volume (ppbv)) was observed in the low-altitude plumes, and also in the upper troposphere where O3 often exceeded 100 ppbv with low aerosol loading. The average tropospheric O3 distributions were determined for the following: Brazil and western South Atlantic, eastern and central South Atlantic, central and east coast of Africa, and the entire South Atlantic Basin. The tropopause heights and O3 columns across the troposphere were calculated for individual flights and for the average O3 distributions in the above regions. A maximum tropospheric O3 column of 56 Dobson units (DU) was found over the biomass burning region in Zambia and in the subsidence region over the central South Atlantic. The high O3 region over the South Atlantic from 4° to 18°S corresponded with the latitudinal extent of the fires in Africa. In situ and laser remote measurements were used to determine the frequency of observation and chemical composition of nine major air mass types. Biomass burning emissions contributed to most of the air masses observed over the South Atlantic Basin, and biomass burning was found to contribute up to half (28 DU) of the O3 column across this region.