A method for the assembly of a thin film containing highly anisotropic colloids that includes the steps of immersing a substrate in a first solution or dispersion comprising a first substance, wherein the first substance has an affinity for the substrate. Then, immersing the substrate in a second solution or dispersion comprising a second substance, wherein the second substance has an affinity for the first substance. A least one of the first substance and the second substance is a highly anisotropic colloid having at least one dimension differing from the others by a ratio of at least 1:1.5. The method incorporates highly anisotropic colloids using a layer-by-layer process that circumvents the tendency for separation of nanotubes at high nanotube loadings. Additionally, the method incorporates aligned highly anisotropic colloids and provides a method for carbon nanotube alignment, which among other advantages makes possible the preparation of unique criss-crossed composites.