We report thin-film transistors (TFTs) capable of controlling mobilities in a broad range using self-assembled nanocomposite multilayers. Single-walled carbon nanotubes (SWNTs) and SiO2 nanoparticles are vertically stacked on a substrate as the semiconducting and dielectric materials, respectively. The number of assembled layers can adjust the nanotube interconnection and tune the mobilities of the transistors. Our experiments show that the mobility can be enhanced to 35 times, and the highest observed mobility is 333.04 cm(2)/V s. Furthermore, we find that the reliability of the devices is increased with the increasing number of SWNT layers in the film. Our results demonstrate an effective technique to produce reliable and high-performance thin-film micro/nanoelectronic devices. Published by Elsevier Ltd.