Selective, template-assisted growth of electrodeposited, layered materials leads to the top-down designable realization of nanopatterned surfaces with a large surface area (>1 cm(2)) comprised of multi-dimensional, multiscale (10 nm-1 μm) features, without the need of standard nanolithography. This process opens a manufacturable route to functional nanodevices that rely on anisotropic, nanoscale surface structures with controlled dimensions.