Radiocaesium introduced to coastal waters by the accident at the Fukushima Dai-ichi Nuclear Power Station (F1NPS) elevated the radioactivity level in biota. The radionuclide level in zooplankton, concentration of 137 Cs radioactivity in surface water fish decreased rapidly, which was the primary food source for planktivorous fish, was recognized as not to be depurated at the same level prior to the accident. To evaluate the possible cause of this phenomenon, zooplankton and surface water fish were collected off Fukushima during 2018-2021, and the presence of radioactive particles was also examined. The concentrations of stable Cs and 137 Cs radioactivity were analysed along with aluminium which was an indicator element of Cs that originated from suspended particles which were attached to or ingested by zooplankton. As a result, radioactive particles were often found in coastal zooplankton samples, and stable Cs and 137 Cs of this inorganic fraction were identified. After removal of this excess radioactivity, the 137 Cs radioactivity in whole-body tissue of zooplankton was derived. However, the level in the soft part of zooplankton during 2018-2020 was still greater than the levels which existed before 2010. Since habitat seawater was understood to not be a substantial source of 137 Cs, then 137 Cs transfer along the food chain, possibly from phytoplankton or detritus of enhanced radioactivity were suggested as important sources of 137 Cs. In addition, enhanced 137 Cs radioactivity in zooplankton was considered consequently elevate radioactivity levels in surface-dwelling water fish off Fukushima. Although the radioactivity level was not radiologically significant in relation to seafood safety limit, enhanced 137 Cs radioactivity levels in biota was demonstrated in southern waters off Fukushima. In contrast, derived 137 Cs/ 133 Cs atom ratios of fish and seawater south of 37°E and west from 142°E indicated that radiocaesium transfer between fish and the environment was in an equilibrium state, showing the environment beyond these geographical coordinates had returned to the pre-accident state.