A method is described for ultrasonically spraying thin films of carbon nanotubes that have been suspended in organic solvents. Nanotubes were sonicated in N-Methyl-2-pyrrolidone or N-Cyclohexyl-2-pyrrolidone and then sprayed onto a heated substrate using an ultrasonic spray nozzle. The solvent quickly evaporated, leaving a thin film of randomly oriented nanotubes. Film thickness was controlled by the spray time and ranged between 200-500 nm, with RMS roughness of about 40 nm. Also described is a method for creating thin (300 nm) conductive freestanding nanotube/polymer composite films by infiltrating sprayed nanotube films with polyimide.