Liquid crystal (LC) molecules have the ability to self-organize into a variety of ordered architectures that are ideal for the design of nanostructured organic materials and investigating the effect of small-scale organization on bulk properties. The focus of our research is the design of polymerizable LCs as a means of forming robust nanostructured polymer materials with enhanced function. One of the goals in this work is the design of LCs that can carry or accommodate polymerization reactivity, as well as an orthogonal functional property of general interest. Through appropriate molecular design, these LC monomers self-assemble into supramolecular assemblies with predictable nanoscale geometries, which are then photopolymerized into robust polymer networks with preservation of their small-scale structures. In this talk, new functional polymer systems based on the cross-linking of lyotropic (i.e., amphiphilic) LCs will be presented. In particular, the inverted hexagonal LC phase containing close-packed cylindrical nanochannels will be presented as one example of this approach. Issues in the design, derivatization, and photopolymerization of functional amphiphilic monomers that adopt this LC architecture will be discussed. The use of the resulting polymers as (1) as size-selective heterogeneous catalysts, and (2) as nanoporous membranes for molecular separations, will be presented. Issues pertaining to the contribution of nanoscale architecture to the performance of these systems will be highlighted. Finally, the design of new lyotropic LC monomer platforms that form phases with a 3-D interconnected nanopore structure (i.e., the bicontinuous cubic phase) around water and room-temperature ionic liquids as the solvent, will be presented.