Anodized aluminum has recently attracted much attention because of its interesting pore structure.[1] The pore structure is a self-ordered hexagonal array of cells with cylindrical pores of variable sizes with diameters of 25±250 nm and with depths exceeding 100 lm depending on the anodizing conditions employed. It can be fabricated through electrochemical anodization of aluminum in various acidic electrolytes, [2±4] and has been demonstrated to provide the basis for an inexpensive, highthroughput fabrication of nanostructures. These properties make anodic aluminum oxide (AAO) a desirable material for many applications, which include microfabricated fluidic devices, [5] quantum-dot arrays, [6±9] magnetic memory arrays, [10] high-aspect-ratio microelectro-mechanical systems, [11] and photonic crystals.[12] The applications of AAO films that have been explored also include template growth of nanotubes, nanowires, creation of nanoholes, nanodots, and nanopillars.[13±15]The ability to pattern porous films is important for a number of technological applications, including sensor arrays, catalysis, optics, and microfluidic devices. Doshi et al. have developed a novel method for patterning mesoporous silica films by employing photosensitive groups.[16] The pore sizes available in such materials are in the range of 2±5 nm, which are small compared to those achievable through anodization of aluminum. Development of patterned AAO membranes, which exhibit high aspect ratio microstructure, is more challenging and the most promising approach for the above mentioned applications. It can be achieved by patterning the aluminum surfaces with an anodization barrier prior to anodization. During anodization of the patterned surfaces, the anodization barrier prevents anodization in the patterned areas while the oxide grows in the unpatterned areas. In addition, it also addresses the fragility problem [17] of AAO membranes due to the presence of aluminum metal that serves as the robust support for nanopore channel arrays. These nanopore channel arrays can then be integrated into microfabricated devices with less fragility problem. Huang et al. [18] have reported the first anodization barrier of poly(methylmethacrylate) deposited on aluminum films. Due to the penetration of the electrolyte through this polymeric layer, the underlying surface was partially anodized to form AAO up to 10 nm deep. In addition, the procedure requires optical lithography, polymer nanoprinting, ionbeam exposure, and milling. Recently, Sun and Kim have reported the formation of alumina nanopore arrays on holographically patterned aluminum films.[19] They patterned aluminum films by using holographic lithography process on silica substrate and anodized the aluminum to get the pores. The pores are not circular and ordered and the pore channels and non-porous substrate are not an integral part of the material. Li et al. [20] and Bae et al. [21] have adopted an indirect method for preparing patterned AAO. First they prepared ordered AAO and patterned the porous ...