The Fukushima Daiichi nuclear power plant accident caused serious radiocesium ( 137 Cs) contamination of forest ecosystems over a wide area. The removal of the forest floor litter layer has been considered a potential method for forest decontamination; however, its effectiveness remains largely unknown. We conducted a pilot-scale decontamination study in a deciduous broadleaved forest in Fukushima. The entire forest was decontaminated by removing the litter layer in July 2014, approximately 3.3 years after the accident, with the exception of two untreated plots. For three years after decontamination, we quantified 137 Cs contamination levels in the litter and topsoil layers and in the tree leaves, in the untreated and decontaminated areas. The decreased inventories of litter materials and the litter-associated 137 Cs in the decontaminated areas were observed only in the first year after decontamination. Generally, no decontamination effects were observed on the 137 Cs transfer in tree leaves. The primary reason for this was the rapid shift in the main reservoir of 137 Cs from litter layers to the underlying mineral soil, which differs from the observations in post-Chernobyl studies of European forest ecosystems. The results suggest that litter-removal decontamination can only be successful if it is implemented more quickly (within 1-2 years after the accident) for Japanese forest ecosystems.The accident at the Fukushima Daiichi nuclear power plant (NPP) in March 2011 released large quantities of radionuclides into the atmosphere 1 and consequently caused serious radioactive contamination of terrestrial ecosystems over a wide area of eastern Japan 2 . Among the radionuclides deposited onto the terrestrial ecosystems, radiocesium ( 137 Cs), with a physical half-life of 30.1 years, is the primary cause for concern because 137 Cs-contaminated ecosystems can increase the radiation exposure to the local population for many years, via both an elevated ambient dose rate in the air (external exposure) and the consumption of contaminated food products (internal exposure) 3 .Decontamination is an important post-accident countermeasure to reduce the radiological impact of a nuclear accident on humans and ecosystems 3,4 . Although since the Fukushima NPP accident, decontamination efforts have been progressing in residential and agricultural areas, forested areas have received a low priority in the decontamination decision-making process, as in the case of the Chernobyl NPP accident 3 , and has not been carried out on a large scale 5 , even though forests provide a wide range of social, cultural, and economic values. This is because the forested areas are vast, occupying approximately 70% of the land in the heavily contaminated area 6 , but are generally not where people live permanently or regularly spend much time. Another reason may be that the forested areas in Japan are concentrated in mountainous and hilly regions with steep terrain, which makes them very sensitive areas to soil erosion. Technical, radiological, and econ...