We have developed a general method for aligning anisotropic materials by using carbon nanotubes to influence order in the surrounding material. Specifically, we have shown that carbon nanotubes seed the formation of oriented domains in a liquid crystalline polymer (LCP). Using polarized light microscopy, we have observed that the molecular alignment in these large (10-100 μm long) domains is homogeneous and controlled by the direction of the nanotube nucleus. The kinetic nature of this nucleation process was verified by differential scanning calorimetry. The coupling of preferential nucleation and controlled seed orientation may allow bulk LCP materials to be aligned by simply preorganizing a small number of dispersed nanotube seeds. We expect that this work will aid in the development and application of macroscopically ordered nanostructured composite materials.