From size considerations alone, polymers and nanoparticles should be natural partners for the preparation of composite materials. However, this prospect is more difficult than first glance would suggest, and clever synthetic, physical, and engineering considerations are required to optimize the merged value of polymers and nanoparticles. In this issue, Jeffrey Pyun and co-workers provide compelling evidence of the value of such composite materials, by stringing together magnetic nanoparticles into "pearl necklace" assemblies. In instructively interdisciplinary fashion, a full complement of polymer chemistry, nanoparticle synthesis, and nanostructural engineering (via solid-phase atomic diffusion) are combined to reveal artistically appealing products with novel properties that hold promise for the future of energy-storage devices and catalytic materials.