Aerosol optical depth measurements were made in October–December 2004 onboard the R/V Akademik Sergey Vavilov. The cruise area included an Atlantic transect from North Sea to Cape Town and then a crossing in the South Atlantic to Argentina. In the open oceanic areas not influenced by continental sources aerosol optical depth values were close to background oceanic conditions (τa ∼ 0.06–0.08). Spectral dependence, especially in the high latitude Southern Atlantic, can be considered as quasi-neutral (Angstrom parameter α was less than 0.4). Back-trajectory analysis allowed statistical division of the aerosol optical parameters and showed similar properties for the North Atlantic polar marine, South Atlantic subtropical marine and South Atlantic polar marine air. Ship-borne aerosol optical depth comparisons to GOCART model and satellite retrievals revealed systematic biases. Satellite retrieved optical depths are generally higher by 0.02–0.07 (depending on the sensor), especially in low τa conditions. GOCART model simulated optical depths correlate well with the ship measurements and, despite overall bias and a notable disparity with the observations in a number of cases, about 30% agree within ±0.01.