processes. Using ion-beam or plasma treatment, many types of nanostructures, such as nanodots, nanobumps, nanopillars, or nanohairs, can be fabricated without any pre-patterning technique. [ 10 ] These nanostructured surfaces have been used in various applications including superhydrophobic coatings, [ 10,11 ] antirefl ective coatings, [ 12 ] controlled bio-adhesion, [ 13 ] and microfl uidic channels. [ 14 ] Recently, many efforts have been focused on investigating the mechanism of nanostructure formation induced by ion-beam or plasma treatment on various polymeric materials. Some reports have suggested that the differential etching behavior of the polymer phase occurs in the crystalline and amorphous states after plasma treatment or dewetting of the surface layer of polymer beads via the effects of plasma energy. [ 9,15 ] Alternatively, the codeposition or incorporation of a third element originating from a vacuum chamber system forms a hard etching inhibitor on the polymeric surfaces. During the oxygen plasma treatment, reactive ion etching not only forms the volatile species, but it also co-deposits the etching inhibitor simultaneously, inducing a large difference in the etching rate. Due to the nature of anisotropic etching during plasma or ion-beam treatment, a roughened surface forms under the ion or plasma beam; the polymeric surface is uniformly etched by the plasma or ion-beam, except for the region with the local metallic clusters, resulting in high-aspect-ratio nanostructures. [ 16,17 ] However, the co-deposited metals may be regarded as undesired third materials on the nanostructured surfaces because the elements that coat the top or sides of the nanostructures might degrade the surface activity during special applications, such as catalysis or sensing. Thus, to prevent the nanostructures from being co-deposited with undesirable metals, sources should be selected using alternative metals. For example, the nanostructures can incorporate functional metallic units, forming a hetero-nanostructure that can be utilized for catalysts, sensors, energy devices, and templates for nanowire growth. [ 4,5,[18][19][20] In this work, we report a simple method for controlling the nanostructure formation on polymeric surfaces by controlling the co-deposition of metals during the oxygen plasma glow discharge. First, we explored the pattern formation induced by oxygen plasma treatment on polyethylene terephthalate (PET); this popular polymer has various applications, Plasma-induced pattern formation is explored on polyethylene terephthalate (PET) using an oxygen plasma glow discharge. The nanostructures on PET are formed through preferential etching directed by the co-deposition of metallic elements, such as Cr or Fe, sputtered from a stainless-steel cathode. The local islands formed by metal co-deposition have signifi cantly slower etching rates than those of the pristine regions on PET, generating anisotropic nanostructures in pillar-or hair-like form during plasma etching. By covering the cathode with the appropriate...