Miniaturization in electronics through improvements in established ™top-down∫ fabrication techniques is approaching the point where fundamental issues are expected to limit the dramatic increases in computing seen over the past few decades. In aspects of biophysics, biotechnology, and diagnostics, nanostructured interfaces are regarded as valuable tools for the localization of individual ligands designed to test single events or for the construction of hierarchical intracellular micro-and nanoarchitectures by the adhesion of cells. [1] Three essential requisites have to be accomplished for these applications: a) the location and connection of nanosized objects with variable distances from subnanometer to submicrometer, b) pattern uniformity over large surface areas or volumes, and c) control of the pattern geometry, including the assembly of asymmetric structures.Principally, the top-down approach addresses dimensions of 50 nm (electron-beam lithography) and larger (photolithography). Smaller dimensions down to 10 nm are feasible by electron-beam lithography, but this involves increased efforts which are economically not viable because they are restricted to small surface areas and low-throughput production. For several years wet-chemistry has provided challenging alternatives to expensive clean-room lithographic techniques. The smallest objects, that is, dots or rods of a few nanometres, are synthesized reproducibly using phases of low-molecular weight surfactants. These objects self-assemble into two-and three-dimensional structures through electrostatic, magnetic, and steric interactions as well as through capillary forces upon evaporation of solvents during film formation. [2,3] The problems arising are the connectivity of the nanoobjects to the macroscopic world, the limited spacings between nanoobjects, and the formation of aperiodic structures. The size range between a few nanometres and 200 nm reflects the gap between top-down approaches and structures made through the pure self-organization of low-molecular-weight species; bridging this size gap offers solutions for overcoming problems of connectivity, breaking pattern symmetry, and noneconomic production aspects. Strategies to bridge this scientific and economically very important size range are addressed through self-assembly of colloidal, [4] macromolecular, [5] or supramolecular units, [6] and thus rely on patterning with periodicities that relate to the molecular weight of the self-organizing molecules. This article presents examples of the latest advances in the application of the selfassembly of macromolecules and colloids, which indeed scale between 5 ± 200 nm, overcome symmetry restriction in selfassembly and substrate choice, and allow for inorganic templating of their structure.Jaeger and co-workers from the University of Chicago demonstrated a method for laterally patterning of metal nanocrystal monolayers onto a solid substrate. [7] In this approach dodecanethiol-ligated gold nanocrystals were synthesized and assembled through both entropic ...