The following research describes the process of fabrication of pentacene films with submicron thickness, deposited by thermal evaporation in high vacuum. The films were fabricated with the aforementioned conditions and their characteristics were analyzed using x-ray diffraction, scanning electron microscopy, polarized Raman spectroscopy, and photoluminescence. Organic thin-film transistors (OTFTs) were fabricated on an indium tin oxide coated glass substrate, using an active layer of ordered pentacene molecules, which were grown at room temperature. Pentacene film was aligned using the ion-beam aligned method, which is typically employed to align liquid crystals. Electrical measurements taken on a thin-film transistor indicated an increase in the saturation current by a factor of 15. Pentacene-based OTFTs with argon ion-beam-processed gate dielectric layers of silicon dioxide, in which the direction of the ion beam was perpendicular to the current flow, exhibited a mobility that was up to an order of magnitude greater than that of the controlled device without ion-beam process; current on/off ratios of approximately 106 were obtained. Polarized Raman spectroscopy investigation indicated that the surface of the gate dielectric layer, treated with argon ion beam, enhanced the intermolecular coupling of pentacene molecules. The study also proposes the explanation for the mechanism of carrier transportation in pentacene films.