Using Metallo-Supramolecular Block Copolymers for the Synthesis of Higher Order Nanostructured Assemblies Adam O. Moughton, Rachel K. O’Reilly* Introduction The desire to control the structure and function of nanostructured materials for use in novel applications has driven scientists to employ a host of synthetic strategies for their creation. [1,2] In particular, the self-assembly of amphiphilic diblock copolymers in solution has facilitated access to various well-defined nanosized architectures. [3–9] For this purpose, typically block copolymers covalently connected at their homopolymer junction are employed, which readily undergo phase separation in a selective solvent for one or more of the homopolymer blocks. This gives rise to various morphologies with typically predictable sizes and shapes, which contain distinct nanosized polymeric domains whose characteristics are defined, and can be tuned by the polymer’s composition and properties. [10–16] Feature Article A. O. Moughton, R. K. O’Reilly Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1DQ, UK E-mail: r.k.o-reilly@warwick.ac.uk A. O. Moughton, R. K. O’Reilly Department of Chemistry, University of Warwick, Gibbet Hill Road, Coventry, CV4 7AL, UK Many research groups have explored the properties and solution self-assembly of main chain metallo-supramolecular multiblock copolymers. Until recently, these metal complexes have been used to prepare mainly micelle type structures. However, the self-assembly of such copolymers has been exploited further to create more advanced architectures which utilize the reversible supramolecular linkage of their building blocks as a key component in their synthesis. Furthermore, the incorporation of multiple orthogonal interactions and stimuli responsive polymers into their design, enables more precise external control of their properties. This feature article discusses recent devel- opments and provides an insight into their potential exploitation and development for the creation of novel, smart, and responsive nano- structures. Macromol. Rapid Commun. 2010, 31, 37–52 ß 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim DOI: 10.1002/marc.200900496 37