The preparation of a new type of cylindrical micelle architecture with an A-B-A triblock structure bearing spatially controlled coronal charge is reported. This was achieved by extending the living supramolecular polymerization approach to block copolymers with hydrophilic blocks and to polar solvents. Electrostatic interactions can be used to selectively functionalize the new nanomaterials with Au and PbS NPs in a spatially selective manner to afford novel composite structures.