We report the unprecedented sergeants and soldiers (S&S)‐type remote control of one‐handed helicity in copolymers of chiral/achiral biphenylylacetylenes bearing amphiphilic oligo(ethylene glycol) (OEG) side chains. A small amount of chiral binaphthyl residues (≤10 mol %) introduced at the terminal of the achiral OEG spacers as many as 80 bonds away from the polymer backbones induced a complete one‐handed helix in water through preferential intramolecular encapsulation of the binaphthyl groups within a cavity of the copolymers. A fully one‐handed helix can be induced virtually independent of the OEG spacer length and concentrations. At a specific spacer length, however, its helix‐sense was inverted. The copolymers also form an excess one‐handed helix in organic solvents in an OEG spacer‐length dependent manner, yet far from the polymer backbones. We show the superiority of the present covalent‐bond driven S&S‐type remote helicity control over the corresponding noncovalent helicity induction approach.

We report the unprecedented sergeants and soldiers (S&S)‐type remote control of one‐handed helicity in copolymers of chiral/achiral biphenylylacetylenes bearing amphiphilic oligo(ethylene glycol) (OEG) side chains. A small amount of chiral binaphthyl residues (≤10 mol %) introduced at the terminal of the achiral OEG spacers as many as 80 bonds away from the polymer backbones induced a complete one‐handed helix in water through preferential intramolecular encapsulation of the binaphthyl groups within a cavity of the copolymers. A fully one‐handed helix can be induced virtually independent of the OEG spacer length and concentrations. At a specific spacer length, however, its helix‐sense was inverted. The copolymers also form an excess one‐handed helix in organic solvents in an OEG spacer‐length dependent manner, yet far from the polymer backbones. We show the superiority of the present covalent‐bond driven S&S‐type remote helicity control over the corresponding noncovalent helicity induction approach.