Developing an efficient and versatile process to transform as ingle linear polymer chain into as hape-defined nanoobject is am ajor challenge in the fields of chemistry and nanotechnology to replicate sophisticated biological functions of proteins and nucleic acids in asynthetic polymer system. In this study,w ep erformed one-shot intrablockc ross-linking of linear blockc opolymers (BCPs) to realizes ingle-chain nanoparticles (SCNPs) with two chemically compartmentalized domains (Janus-shaped SCNPs). Detailed structural characterizations of the Janus-shaped SCNP composed of polystyreneblock-poly(glycolic acid) revealed its compactly folded conformation and compartmentalized blockl ocalization, similar to the self-folded tertiary structures of natural proteins. Versatility of the one-shot intrablockc ross-linking was demonstrated using several different BCP precursors.I na ddition, the Janus-shaped SCNP produce miniscule microphase-separated structures.

Developing an efficient and versatile process to transform a single linear polymer chain into a shape‐defined nanoobject is a major challenge in the fields of chemistry and nanotechnology to replicate sophisticated biological functions of proteins and nucleic acids in a synthetic polymer system. In this study, we performed one‐shot intrablock cross‐linking of linear block copolymers (BCPs) to realize single‐chain nanoparticles (SCNPs) with two chemically compartmentalized domains (Janus‐shaped SCNPs). Detailed structural characterizations of the Janus‐shaped SCNP composed of polystyrene‐block‐poly(glycolic acid) revealed its compactly folded conformation and compartmentalized block localization, similar to the self‐folded tertiary structures of natural proteins. Versatility of the one‐shot intrablock cross‐linking was demonstrated using several different BCP precursors. In addition, the Janus‐shaped SCNP produce miniscule microphase‐separated structures.