The redox switchable formation of very well-defined supramolecular graft polymers in aqueous solution driven by host-guest interactions between ferrocene (Fc) and cyclodextrin (CD) is presented. The Fc-containing acrylic backbone copolymer (PDMA-stat-Fc) is prepared via reversible addition-fragmentation chain transfer (RAFT) copolymerization of N, N-dimethylacrylamide (DMA) and the novel monomer N-(ferrocenoylmethyl) acrylamide (NFMA). Via the RAFT process, copolymers containing variable Fc ratios (5-10 mol%) are prepared, affording polymers of molecular masses of close to 11 000 g mol(-1) and molar mass dispersities (D) of 1.2. The beta-cyclodextrin (beta-CD) containing building block is synthesized via RAFT-polymerization, too, in order to afford a polymer with well-defined molecular mass and low dispersity ((M) over bar (n) = 10 300 g mol(-1), D = 1.1), employing a propargyl-functionalized chain transfer agent for the polymerization of N, N-diethylacrylamide (DEA). The polymerization product is subsequently terminated with beta-CD via the regiospecific copper (I)-catalyzed 1,3-cycloaddition (PDEA-beta CD). Host-guest interactions between Fc and CD lead to the formation of supramolecular graft-polymers, verified via nuclear Overhauser enhancement spectroscopy (NOESY). Importantly, their redox-responsive character is clearly confirmed via cyclic voltammetry (CV). The self-assembly of the statistical Fc-containing lateral polymer chain in aqueous solution leads to mono-and multicore micelle-aggregates evidenced via TEM. Only diffused cloud-like, non-spherical nanostructures are observed after addition of PDEA-beta CD (TEM).