A reliable surface treatment for the pentacene/gate dielectric interface was developed to enhance the electrical transport properties of organic thin-film transistors (OTFTs). Plasma-polymerized fluorocarbon (CFx) film was deposited onto the SiO2 gate dielectric prior to pentacene deposition, resulting in a dramatic increase of the field-effect mobility from 0.015 cm(2)/(V s) to 0.22 cm(2)/(V s), and a threshold voltage reduction from -14.0 V to -9.9 V. The observed carrier mobility increase by a factor of 10 in the resulting OTFTs is associated with various growth behaviors of polycrystalline pentacene thin films on different substrates, where a pronounced morphological change occurs in the first few molecular layers but the similar morphologies in the upper layers. The accompanying threshold voltage variation suggests that hole accumulation in the conduction channel-induced weak charge transfer between pentacene and CFx. (C) 2008 Elsevier B.V. All rights reserved.