An inkjet printing procedure for depositing films of carbon nanotubes (CNTs) that exhibit a very high degree of long-range mutual alignment as well as a controlled orientation with respect to the printed geometry is presented. CNT self-assembly was induced by the intrinsic lyotropic liquid crystallinity of CNT suspensions. Sufficient concentrations are reached by matching the inkjet deposition rate to the numerically modeled local evaporation rate of the printed feature and enable the CNT suspension to be printed using standard inkjet printing. Surface alignment was verified using scanning electron microscopy (SEM) and polarized light microscopy. In addition, the bulk morphology was investigated and found to be composed of stacked planar layers that did not necessarily have the same long-range orientation found on the surface. The bulk morphology was characterized by removing layers through an elastomeric peeling process and by observing cross sections of the films using SEM. CNT concentration and length were spanned experimentally, and it was found that very short and very long CNTs as well as low concentration suspensions did not yield long-range alignment.