A system for simulating aerosols has been developed using a chemical transport model together with an assimilation of satellite aerosol retrievals. The methodology and model components are described in this paper, and the modeled distribution of aerosols for the Indian Ocean Experiment (INDOEX) is presented by Rasch et al. [this issue]. The system generated aerosol forecasts to guide deployment of ships and aircraft during INDOEX. The system consists of the Model of Atmospheric Transport and Chemistry (MATCH) combined with an assimilation package developed for applications in atmospheric chemistry. MATCH predicts the evolution of sulfate, carbonaceous, and mineral dust aerosols, and it diagnoses the distribution of sea salt aerosols. The model includes a detailed treatment of the sources, chemical transformation, transport, and deposition of the aerosol species. The aerosol forecasts involve a two-stage process. During the assimilation phase the total column aerosol optical depth (AOD) is estimated from the model aerosol fields. The model state is then adjusted to improve the agreement between the simulated AOD and satellite retrievals of AOD. During the subsequent integration phase the aerosol fields are evolved using meteorological fields from an external model. Comparison of the modeled AOD against estimates of the AOD from INDOEX Sun photometer data show that the differences in daily means are -0.03 ± 0.06. Although the initial application is limited to the Indian Ocean, the methodology could be extended to derive global aerosol analyses combining in situ and remotely sensed aerosol observations. Copyright 2001 by the American Geophysical Union.