Application of pulsed high negative voltage (∼10 μs pulse width, 300–900 pulses per second) to a substrate is found to induce discharge, thereby increasing ion current with an inductively coupled plasma source. This plasma source ion beam implantation (PSII) technique is investigated for the pretreatment and deposition of diamond-like carbon (DLC) thin layer on polyethylene terepthalate (PET) film. Pretreatment of PET with N2 and Ar plasma is expected to provide added barrier effects when coupled with DLC deposition, with possible application to fabrication of PET beverage bottles. PSII treatment using N2 and Ar in separate stages is found to change the color of the PET film, effectively increasing near-ultraviolet absorption. The effects of this pretreatment on the chemical bonding of C, H, and O are examined by x-ray photoelectron spectroscopy (XPS). DLC thin film was successfully deposited on the PET film. The surface of the DLC thin layer is observed to be smooth by scanning electron microscopy, and its structure characteristics are examined by XPS and laser Raman spectroscopy. Subsequent processing using acetylene or acetylene and Ar (20%) produced thin carbon layers that are confirmed to be graphite-dominated DLC. Also, this PSII method is employed in order to deposit the DLC layer on the inside surface of the PET bottle and to reduce oxygen permeation rate by 40%. © 2002 American Vacuum Society.