We present the results of aerosol forecast during the ACE-Asia field experiment in spring 2001, using the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model and the meteorological forecast fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). The model provides direct information on aerosol optical thickness and concentrations for effective flight planning, while feedbacks from measurements constantly evaluate the model for successful model improvements. We verify the model forecast skill by comparing model-predicted aerosol quantities and meteorological variables with those measured by the C-130 aircraft. The GEOS DAS meteorological forecast system shows excellent skills in predicting winds, relative humidity, and temperature, with skill scores usually in the range of 0.7–0.99. The model is also skillful in forecasting pollution aerosols, with most scores above 0.5. The model correctly predicted the dust outbreak events and their trans-Pacific transport, but it constantly missed the high dust concentrations observed in the boundary layer. We attribute this “missing” dust source to desertification regions in the Inner Mongolia Province in China, which have developed in recent years but were not included in the model during forecasting. After incorporating the desertification sources, the model is able to reproduce the observed boundary layer high dust concentrations over the Yellow Sea. We demonstrate that our global model can not only account for the large-scale intercontinental transport but also produce the small-scale spatial and temporal variations that are adequate for aircraft measurements planning.