The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident caused a significant release of radionuclides into the environment. It is important to explore the timing and amount of radioactive release to terrestrial areas in order to clarify the consequences of the accident, including the dose received by the population living in the areas affected by the accident. In general, backward estimations are performed using air concentrations of radionuclides, but they are difficult to measure when radioactive plumes are passing through, and only spatially and temporally limited measurements are available. Therefore, a new method of backward estimation was developed based on the total cumulative deposition density, which can provide sufficient data in the environment by combining the atmospheric transport, dispersion, and deposition model calculations. Consequently, our estimations show that a major release of 137Cs and 131I occurred on 15, 20, 21, 22, 25, and 30 March 2011, after the accident. The amounts of release estimated by our new method for 137Cs and 131I were 4.9 × 1015 Bq and 120 × 1015 Bq, respectively. These results have no significant contradiction with the estimated results by the previous studies that were based on air concentrations and air dose rates that were measured in terrestrial areas. It was found that our new method is applicable for backward estimation oriented to the dose assessment for the people living in terrestrial areas.