In this chapter, bottom-up strategies for fabricating nanoscale ring structures to produce optical metamaterials are described. Co-assemblies of submicrometer-sized spherical polymer particles and metal nanoparticles spontaneously form three-dimensional (3D) nano-ring arrays among polymer particles through self-assembly of metal nanoparticles at the evaporation meniscus. Colloidal assemblies of submicrometer particles, which form 3D periodic structures, are used as templates to assemble metal nanoparticles and block copolymers. Block copolymers form phase-separated structures tens of nanometers in size; thus, metal nanoparticles can be self-assembled into the phase-separated block copolymers. These bottom-up methodologies are useful for fabricating optical metamaterials.