With the increasing appeal of nanotechnology, there is a demand for development of synthetic techniques for the fabrication of nanosized objects that allow for precise size control and tailored functionalization. To this end, the collapse or folding of single polymer chains into architecturally defined nanostructures is a rapidly growing research topic in polymer science. Many synthetic approaches have been developed for the formation of single-chain nanoparticles (SCNP), and a variety of characterization methods and computational efforts have been utilized to detail their formation and probe their morphological characteristics. Interest in this field continues to grow partially due to the variety of potential applications of SCNP including catalysis, sensors, nanoreactors, and nanomedicine. While numerous developments have been made, the field is continuing to evolve, and there are still many unanswered questions regarding synthesis and characterization of SCNP. This Perspective serves to identify recent accomplishments in the synthesis and characterization of SCNP while distinguishing areas that are in need of advancement and innovation to move forward. This includes exploring more complex synthetic strategies, obtaining folding control, employing nanoparticle functionalization, developing scalable methods, investigating hierarchical self-assembly of SCNP, and exploiting unique characterization techniques and in-depth simulations.