The construction of nanostructured objects of well-defined size is of outmost importance for nanotechnology to surmount claims for potential applications and exploit improved chemical, physical or biological properties of a functional nanofeatured material. Biomedical imaging is one particular field of interest for water-compatible chemical self-assembly of nanosized objects. The outlined project aims to develop a methodology for the preparation of nanostructured objects in aqueous media with the emphasis lying on the precise control over the size, shape and degree of functionalisation of the features. The goal is to build upon supramolecular helical scaffolds for the development of self-assembled functional structures in the nanoscopic range, which are to be used in magnetic resonance imaging (MRI) applications. MRI has made a significant impact to the area of diagnostic medicine, predominantly due to advances in the development of contrast agents (e.g. paramagnetic Gd(III)-complexes). We believe that a supramolecular approach based on self-assembled Gd(III) chelating molecular units can combine the benefits from both low and high molecular weight derivatives: high contrast agent efficiency or contrast enhancement on one hand, and an improved control over the pharmacokinetics on the other hand, because of the non-covalent dynamic nature that holds the objects together. Furthermore, challenges in the field of MRI contrast agents will be met by the development of multivalent target-specific structures. Advantages include the accumulation of MRI signals in a region of interest, and the combination of 1H MRI contrast enhancement with a second imaging label. 19F MRI is a highly promising probe because of the high sensitivity of the 19F nuclide and the absence of any background interference in living systems.