The volatile nuclides, 131I, 132I, and 132Te, which were released in large quantities during the early stage of the Fukushima Dai-ichi Nuclear Power Plant accident, are the most dominant ones in determining the impact on the public and the environment. Since the behavior of these nuclides in the environment and their effects on human health differ depending on their physicochemical forms, it is necessary to understand more about the release fraction and the deposition process of each form. In this study, a behavior model was developed to calculate physical and chemical processes of organic, inorganic, and particulate 131I and 132I, and gaseous and particulate 132Te. This behavior model was used to estimate the physicochemical composition of iodine at the time of release, the 132Te/132I activity ratio at the time of release, and the dry deposition velocity of 132Te. The estimation was performed for five plumes transported during the period from March 14 to 21, 2011, and the estimated values were obtained by comparing with the values measured in previous studies. As a result of the estimation, the organic iodine fraction at the time of release was estimated to be 0.1 or less for most plumes, while a significantly higher value of 0.3 was estimated for the plume released in the night of March 14. This result implied that the possibility of formation and release of organic iodine in the liquid phase in Unit 3, which was considered to be the source of this plume. As for the 132Te/132I ratio at the time of release, it was estimated to be about 0.3–0.4 for most plumes, while it was about 1 in the plume released in the early morning of March 15, which is consistent with the release process in Unit 2 on the night of 14 and early morning of the 15. In addition, a remarkably high dry deposition velocity of 132Te was estimated in this plume, which was consistent with the existence of radiocaesium-bearing microparticles (CsMP) with a particle size of a few micrometers that had been found to be specific to this plume.