Global simulations of the composition of and direct forcing due to aerosols containing natural and/or anthropogenic sulfate, nitrate, chloride, carbonate, ammonium, sodium, calcium, magnesium, potassium, black carbon, organic matter, silica, ferrous oxide, and aluminum oxide were carried out. Chloride and natural sulfate were found to be the most important natural aerosol constituents in the atmosphere in terms of solar plus thermal-infrared forcing. Sea spray was the most important natural aerosol type, indicating that it should be accounted for in weather and climate calculations. Ammonium was found to have a positive direct forcing, since it reduces water uptake in sulfate-containing solutions; thus, anthropogenic ammonium contributes to global warming. The magnitudes of ammonium and nitrate forcing were smaller than those of chloride or sulfate forcing. When organics were divided into three groups with different assumed UV absorption characteristics, total aerosol direct forcing at the tropopause increased by about +0.03 to +0.05 W m-2 (direct forcing by organics remained negative), suggesting that UV absorption by organics is a nontrivial component of the global energy balance. Gypsum <CaSO4-2H2O>, sal ammoniac <NH4Cl>, halite , halite, and nitrum <KNO3> were estimated to be the most common sulfate-, ammonium-, sodium-, chloride-, and nitrate-containing solid-phase aerosol constituents, respectively, in the global atmosphere. Solid formation in aerosols was found to increase total-aerosol direct forcing by +0.03 to +0.05 W m-2. Spatial and vertical forcing estimates, sensitivities of forcing to relative humidity and concentration, and estimates of global aerosol liquid water content are given. Modeled aerosol optical properties are compared with satellite and field measurements. ¿ 2001 American Geophysical Union