The invention is directed to carbon nanostructure composite systems which may be useful for various applications, including as dry adhesives, electronics and display technologies, or in a wide variety of other areas where organized nanostructures may be formed and integrated into a flexible substrate. The present invention provides systems and methods wherein organized nanotube structures or other nanostructures are embedded within polymers or other flexible materials to provide a flexible skin-like material, with the properties and characteristics of the nanotubes or other nanostructures exploited for use in various applications. In one aspect, the invention is directed to a carbon nanotube/polymer composite material having a plurality of carbon nanotubes formed into a predetermined architecture, with each of the plurality of nanotubes having a desired width and length. The architecture of the plurality of nanotubes defines at least one orientation for a plurality of nanotubes, and also defines the approximate spacing between nanotubes and/or groups of nanotubes. The carbon nanotube architecture is at least partially embedded with a polymer matrix in a manner that the architecture is stabilized in the predetermined architecture. The polymer matrix may also be formed to have a desired predetermined thickness.