As a part of the Global Change Expedition/Coordinated Air-Sea Experiment/Western Atlantic Ocean Experiment (GCE/CASE/WATOX), size distributions of marine aerosols were measured at two altitudes of about 2750 and 150 m above sea level (asl) over the size range 0.1 ∼ 32 μm. Lognormal fitting was applied to the corrected aerosol size spectra to determine the volume and surface area size distributions of the CASE-WATOX marine aerosols. Each aerosol size distribution was fitted with three lognormal distributions representing fine-, large-, and giant-particle modes. Water volume fraction and dry particle size of each aerosol size distribution were also calculated using empirical formulas for particle size as a function of relative humidity and particle type. Because of the increased influence from anthropogenic sources in the continental United States, higher aerosol volume concentrations were observed in the fine-particle mode near-shore off the east coast; 2.11 and 3.63 μm3 cm−3 for free troposphere (FT) and marine boundary layer (MBL), compared with the open-sea Bermuda area values; 0.13 and 0.74 μm3 cm−3 for FT and MBL. The large-particle mode exhibits the least variations in volume distributions between the east coast and open-sea Bermuda area, having a volume geometric median diameter (VGMD) between 1.4 and 1.6 μm and a geometric standard deviation between 1.57 and 1.68. For the giant-particle mode, larger VGMD and volume concentrations were observed for marine aerosols nearshore off the east coast than in the open-sea Bermuda area because of higher relative humidity and higher surface wind speed conditions. Wet VGMD and aerosol water volume concentrations at 15 m asl ship level were determined by extrapolating from those obtained by analysis of the CASE-WATOX aircraft aerosol data. Abundance of aerosol water in the MBL serves as an important pathway for heterogeneous conversion of SO2 in sea salt aerosol particles.