The general approach involving the organization of polymers into micellar assemblies followed by stabilization through covalent intramicellar crosslinking of the assemblies has emerged as a powerful method for the production of well-defined nanostructured materials, having an amphiphilic core-shell morphology. When the covalent crosslinks are limited to chain segments that compose the polymer micelle shell, then shell crosslinked knedel-like (SCK) nano-structures result. The shell composition dictates the interactions of the SCKs with external agents, forms a barrier layer over the core domain, and provides robust character to the nanoparticle. Because of the stability that the crosslinked shell provides, the core domain can be of dramatically different compositions and properties-glassy, fluidlike, and crystalline polymer chains have been employed for the core material and the effects that each contributes to the overall nano-structure properties have been examined. Most notably, the shell crosslinks allow for complete removal of the core to generate hollow (solvent-filled) nanoscale cagelike structures.