The Fukushima Dai-ichi nuclear power plant (FNPP) accident that followed the Great East Japan Earthquake in 2011 resulted in the release of enormous quantities of anthropogenic radionuclides, especially radioactive cesium (134Cs and 137Cs) into the ocean off the east coast of Japan. FNPP-derived radioactive Cs may have consequently accumulated within marine food webs via seawater intake and predator–prey interactions. We provide evidence of the temporal variability in 134Cs and 137Cs concentrations in seawater and zooplankton samples collected in coastal waters off Joban-Sanriku, in Sendai Bay, and in the Oyashio region between June 2011 and December 2013. In Sendai Bay, seawater 134Cs and 137Cs concentrations exceeded 1 Bq/kg in June 2011 and rapidly decreased during the study period. 134Cs and 137Cs concentrations in zooplankton were also high in June 2011, up to 23 Bq/kg-wet and also decreased during the study period, although at a slower rate than seawater 134Cs and 137Cs concentrations. Regarding 137Cs concentrations, the difference in the rate of decrease between seawater and zooplankton resulted in a high apparent concentration ratio (aCR) for zooplankton. The observed relation between 137Cs in seawater and the aCR of zooplankton were good indicators of the progress of 137Cs contamination in zooplankton from the beginning of the FNPP accident to the restoration phase.