Forest-stream ecotones possess prominent detritus-based food webs, and 137Cs-contaminated litter can influence the contamination levels of animals inhabiting such ecosystems. The effects of leaching on contaminated litter induce greater absolute differences between the 137Cs concentrations of forest and stream litter in more contaminated sites. Because 137Cs concentrations in litter can be attenuated temporally, spatiotemporal patterns in the differences in 137Cs concentrations between forest and stream litter may vary depending on both the amount of 137Cs deposition and the passage of time. To test this hypothesis, we sampled coniferous needle and broad-leaved deciduous litter in forests and streams at seven forested headwater sites affected by the Fukushima nuclear accident 3.24 and 11.24 years after the accident. We found that 137Cs concentrations in the two litter types were one order of magnitude lower 11.24 years after the accident than 3.24 years afterwards. The absolute difference in 137Cs activity concentrations of litter between forest and stream ecosystems was higher at more contaminated sites both 3.24 and 11.24 years after the accident. The spatiotemporal changes in litter contamination provide insight into 137Cs dynamics and complex transfer in the detritus-based food webs of forest-stream ecotones.