In this paper, organic electroluminescence fluoropolymer film devices, i.e., organic light-emitting diodes (OLEDs) comprising polychlorotrifluoroethylene (PCTFE) films treated by an atmospheric-pressure nonthermal plasma (NTP) graftpolymerization process, are investigated. PCTFE films can provide a long lifetime for OLEDs because of their excellent gas barrier properties; however, they are difficult to laminate, owing to low adhesiveness. The surfaces of PCTFE films are treated by an atmospheric-pressure NTP-graft-polymerization process to improve their adhesiveness, and then, indium tin oxide and a luminous layer are deposited on the treated PCTFE films. As a result, OLEDs comprising PCTFE films are successfully demonstrated.