Hydrogenated amorphous carbon (a-C:H) films have been deposited on poly(ethylene terephthalate) (PET) films with an pulse-biased inductively coupled plasma chemical vapor deposition method using CH 4 and C 2 H 2 gases. We have investigated the effects of the pulse-bias frequency on the oxygen transmission rate (OTR) of the a-C:H-coated PET sample, and discussed relationship between the OTR characteristics and the structure of the films based on the results of Raman and infrared absorption spectroscopy. In case of CH 4 plasmas, the OTR of the sample has been reduced down to 1.12 cm 3 /(m 2 ÁdayÁatm) by increasing the bias-frequency to 2 kHz, and the structure of the a-C:H films has been modified from polymer-like to tetrahedral one. In case of C 2 H 2 plasmas, the OTR of the samples has been 1.18 cm 3 /(m 2 ÁdayÁatm) with the lower bias frequency of 0.5 kHz, and has not shown strong dependence on the pulse-bias frequency. This has been explained by the fact that the films prepared with C 2 H 2 plasma can be modified to tetrahedral structures by applying the bias with the lower frequency. #