Well‐aligned carbon nanowalls with a thickness of a few nanometers and a lateral size in the micrometer range have been grown on various types of substrates. The nanowalls exhibit a remarkably different surface morphology as compared to fullerenes and carbon nanotubes, in particular their two‐dimensionality and high surface area. In this work, we focused on the second aspect and developed a templating method to fabricate a class of nanostructured materials based on the novel surface morphology of the carbon nanowalls. These structures may have potential applications in batteries, gas sensors, catalysts, and light‐emission/detection, field‐emission, and biomedical devices.