Among the many phenomena revealed and provided by nanoscience, the functionalization of a surface by nanopatterning certainly holds promise for a large number of attractive applications. A prominent example is the deposition of self-assembled monolayers by microcontact printing in order to control wettability, adhesion, friction, and wear. [1,2] In this context, the well-known lotus effect should be mentioned. This effect is based on a strong reduction of the adhesion of water droplets by nanopatterning a surface with, for example, dense arrays of statistically distributed nanopillars. [3,4] A further application of such nanopillars is their use as effective electron field emitters, as has been demonstrated for Si, [5,6] a material which is also at the focus of the present work, or, more recently, for diamond. [7] Moreover, highly ordered arrays of nanopillars are extremely helpful for the characterization of individual emitters by scanning tunneling microscopy (STM) or scanning tunneling spectroscopy (STS).For an inverted pattern of nanopillars, that is, ordered arrays of cylindrical nanopores with a high aspect ratio, a similar wealth of possible applications can be thought of. For instance, they can serve as contact holes in semiconductors. According to the present semiconductor technology roadmap, they should exhibit diameters well below 80 nm for the "65 nm node generation".[8] Similarly, applications in nanooptics appear attractive; nanopores based on colloidal masks were fabricated into Si with a diameter of 60 nm. [9] Smaller diameters of the order of 30 nm should be obtainable by nanomachining a poly(methyl methacrylate) PMMA resist with an atomic force microscope and subsequent metal-coating and lift-off, thereby accepting the disadvantage of a nonparallel process. [10] Note that the recently developed technique of controlling the diameter of nanopores in ultrathin Si/SiO 2 membranes by the electron beam of a transmission electron microscope is still a nonparallel procedure.[11] Another approach to preparing nanoholes in Si is based on self-organized porous alumina masks in combination with anisotropic Cl 2 reactiveion etching (RIE). [12] In this way, holes with diameters > 13 nm and an aspect ratio of 3 could be obtained. Similar diameters are obtained by a recently reported technique based on the self-organization of inverse spherical micelles formed from diblock copolymers dissolved in an apolar solvent, such as toluene, and selectively loaded in the micellar core with a metal salt, such as HAuCl 4 .[13-16] By dip-coating such solutions onto practically any sufficiently flat substrate, hexagonally ordered arrays of Au nanodots can be prepared by an ashing process.[17] They can be used as nanomasks in a subsequent anisotropic etching step, resulting in corresponding arrays of nanopillars. In this way, hexagonally ordered pillars with a diameter of 14 nm and an aspect ratio of 5 were obtained in Si. This micellar preparation technique offers a number of impressive advantages, such as the control of the...