Between 1944 and 1956, radioactive 131I was released into the atmosphere from operations at the Oak Ridge National Laboratory in Oak Ridge, TN. The releases occurred from stacks and from building vents and openings in three different chemical forms: elemental, organic, and particulate. During their transport in the atmosphere, different forms of iodine react differently with other atmospheric chemicals and moisture, and are removed from the plume at different rates by the processes of dry and wet deposition. A modified Gaussian plume model was developed to address the processes of radioiodine speciation, deposition, depletion, and dispersion in the atmosphere, and to propagate uncertainties in input parameter values through to the ground-level concentrations of 131I in air. A unique approach was used to develop an implicitly correlated set of hourly meteorological parameters for any day of a month for each month of the year from ten years of available data between 1987 and 1996. The model was validated for both annual average and short-term releases. For the annual average releases, the predictions of ground-level concentrations of 131I from the model were within a factor of 2 of measured field data. For two of the three sets of available weekly data, the measurements fell within the 95% subjective confidence interval of model predictions. Predictions of ground-level air concentrations were made on an annual average basis for the entire period of release and on a short-term, episodic basis for a 1954 accident.