Thin films of carbon nanotubes (CNTs) are fabricated from solution using a one-step directed assembly strategy. Very high surface selectivity and exceptionally high CNT densities can be observed in small features with complex shapes. This directed assembly technique makes use of minimum amounts of CNTs and low toxicity solvents, and can be applied to metallic, semiconducting and mixed CNTs for fabrication of thin films over macroscopic areas. The thin films obtained with this approach are used for thin-film transistor (TFT) fabrication, and their electrical characterization is described. © 2014 American Chemical Society.