Aerosol carbon concentrations, organic / elemental speciation, and carbon isotopic composition data (13C/12C ratios and 14C content) are reported from the second Rio de Janeiro Aerosol Characterization Study (RIO-JACS II), along with supplemental meteorologic and inorganic aerosol data. These data and their diurnal and weekday / weekend variability are used to identify sources of carbonaceous aerosols in the urban Rio air basin. Specifically, contributions from biogenic sources, anthropogenic emissions (principally transportation sources), and sugar cane-derived alcohol-fueled vehicular emissions to aerosol carbon levels in Rio are estimated from measurements of carbon-14, organic and elemental carbon, and 13C/12C isotopic composition in total aerosol samples collected at two ambient Rio sites and in a heavily traveled tunnel. The major source of elemental (soot) carbon appears to be diesel vehicles, but secondary sources of both biogenic and fossil organic aerosol carbon are indicated.