Water samples collected along the Japanese coast and in the open Pacific Ocean in 2010, 2011, and 2012 were analyzed for perfluoroalkyl substances (PFASs) to evaluate the effect of Great East Japan Earthquake (EQ 3.11), which occurred on March 11, 2011, on the dispersion of chemical pollutants. Ultratrace analysis of PFASs in water, a super computer simulation, and an inventory analysis from industrial records revealed the sources and dynamics of PFASs during the EQ 3.11 disaster. In this respect, EQ 3.11 destroyed solid infrastructure on land, and within minutes, PFASs stocked therein were released into the open environment. The historically significant tsunami backwash swept them away from their origin to the coastal water within several hours. It was estimated that from 0.8 to 1.0 tons of perfluorooctanesulfonate (PFOS) and 4.8 to 5.1 tons of PFOA were discharged into the coastal waters after EQ 3.11 and the tsunami that followed. The reconstruction of EQ 3.11 also traced the influence of this pollution in open ocean water until March 2012, and a statistical and finger printing analysis revealed that there were different distribution mechanisms in coastal regions than in the open ocean for PFOS, other shorter chain perfluorinated sulfonic acids and perfluorinated carboxylic acids.