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The development of high-dielectric-constant polymers as active materials in high-performance devices is one of challenges in polymer-based electric system like flexible high-energy-density capacitors and organic thin-film transistors. Here, we incorporated homochiral (1S)-(+)-10-camphorsulfonic acid (CSA) and non-linear optical Disperse Yellow 7 (DY7) into poly (2-vinylpyridine)-block-poly (methyl methacrylate)(P2VP-b-PMMA) copolymers via both ionic interactions and hydrogen bonding, forming a supramolecular assembly with cylindrical nanostructures. In contrast to the P2VP homopolymer assembly with a dielectric constant less than 10 at room temperature, supramolecular diblock copolymer assembly exhibits a temperature-and frequency-independent dielectric constant close to 50 at frequencies lower than 100 Hz. This is comparable with that of ferroelectric poly (vinylidene fluoride-trifluoroethylene …