We measured carbonaceous material and water-soluble ionic species in the fine fraction (Dp < 1.3 ¿m) of aerosol samples collected on NCAR's C-130 aircraft during the intensive field phase (February--March 1999) of the Indian Ocean Experiment (INDOEX). Polluted layers were present over most of the study region north of the equator at altitudes up to 3.2 km. The estimated aerosol mass (sum of carbonaceous and soluble ionic aerosol components) of fine-mode particles in these layers was 15.3 ¿ 7.9 ¿g m-3. The major components were particulate organic matter (POM, 35%), SO42- (34%), black carbon (BC, 14%), and NH4+ (11%). The main difference between the composition of the marine boundary layer (MBL, 0 to ~1.2 km), and the overlying residual continental boundary layer (1.2 to ~3.2 km) was a higher abundance of SO42- relative to POM in the MBL, probably due to a faster conversion of SO2 into SO42- in the MBL. Our results show that carbon is a major, and sometimes dominant, contributor to the aerosol mass and that its contribution increases with altitude. Low variability was observed in the optical properties of the aerosol in the two layers. Regression analysis of the absorption coefficient at 565 nm on BC mass (BC < 4.0 ¿g C m-3) yielded a specific absorption cross section of 8.1 ¿ 0.7 m2 g-1 for the whole period. The unusually high fraction of BC and the good correlation between the absorption coefficient and BC suggest that BC was responsible for the strong light absorption observed for the polluted layers during INDOEX. High correlation between BC and total carbon (TC) (r2 = 0.86) suggest that TC is predominantly of primary origin. Good correlations were also found between the scattering coefficient at 550 nm and the estimated aerosol mass for the fine fraction. These yielded a specific scattering cross section of 4.9 ¿ 0.4 m2 g-1. The observed BC/TC, BC/OC, SO42-/BC, and K+/BC ratios were fairly constant throughout the period. These ratios suggest that between 60 and 80% of the aerosol in the polluted layers during INDOEX originated from fossil fuel and between 20 and 40% from biofuel combustion.