Thin film transistors (TFTs) are now poised to revolutionize the display, sensor, and flexible electronics markets. However, there is a limited choice of channel materials compatible with low-temperature processing. This has inhibited the fabrication of high electrical performance TFTs. Single-walled carbon nanotubes (CNTs) have very high mobilities and can be solution-processed, making thin film CNT-based TFTs a natural direction for exploration. The two main challenges facing CNT-TFTs are the difficulty of placing and aligning CNTs over large areas and low on/off current ratios due to admixture of metallic nanotubes. Here, we report the self-assembly and self-alignment of CNTs from solution into micron-wide strips that form regular arrays of dense and highly aligned CNT films covering the entire chip, which is ideally suitable for device fabrication. The films are formed from pre-separated, 99% purely semiconducting CNTs and, as a result, the CNT-TFTs exhibit simultaneously high drive currents and large on/off current ratios. Moreover, they deliver strong photocurrents and are also both photo- and electroluminescent.