A three-dimensional aerosol transport-radiation model coupled with a general circulation model, Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS), simulates atmospheric aerosol distributions and optical properties. The simulated results are compared with aerosol sampling and optical observations from ground, aircraft, and satellite acquired by intensive observation campaigns over east Asia in spring 2001. Temporal variations of the aerosol concentrations, optical thickness, and Ångström exponent are in good agreement between the simulation and observations. The midrange values of the Ångström exponent, even at the Asian dust storm events over the outflow regions, suggest that the contribution of the anthropogenic aerosol, such as carbonaceous and sulfate, to the total optical thickness is of an order comparable to that of the Asian dust. The radiative forcing by the aerosol direct and indirect effects is also calculated. The negative direct radiative forcing is simulated to be over −10 W m⁻² at the tropopause in the air mass during the large-scale dust storm, to which both anthropogenic aerosols and Asian dust contribute almost equivalently. The direct radiative forcing, however, largely depends on the cloud water content and the vertical profiles of aerosol and cloud. The simulation shows that not only sulfate and sea salt aerosols but also black carbon and soil dust aerosols, which absorb solar and thermal radiation, make strong negative radiative forcing by the direct effect at the surface, which may exceed the positive forcing by anthropogenic greenhouse gases over the east Asian region.