In the current issue of ACS Nano, Lobling, Haataja et al. craft polymeric nanoparticles with a hierarchy of nontrivial surface structures by combining conventional interpolyelectrolyte complexation with steric control from an uncharged copolymer block. Remarkable cylindrical and lamellar nanodomains are produced on the polyionic coronae of spherical micelles. Here, we discuss generalizing this elegant self-assembly strategy and provide speculative perspectives for its future potential for new nanomaterials.