The unique structural, mechanical, and electronic properties of carbon nanotubes (CNTs) have resulted in their development into a standard material for a variety of applications. In particular, CNTs have been widely investigated for electronic applications, which include use as transistors, [1] photovoltaic devices, [2] active sensing elements, [3] and building blocks for biosensors. [4] One of the main challenges currently involves assembling CNTs on a substrate in a manner that allows the secondary association of redox-active components to the CNTs and rapid electron transfer along the tubes. [4a] To this end, functional groups are formed at the CNT edges in order to ensure stable anchoring. [5,6] Alternative routes exploit the physical adsorption of either hydrophilic groups [7] or watersoluble polymers on the CNT walls. [8] Although polymercoated CNTs were used for the functionalization of different surfaces, [8] this method has severe limitations when fabricating highly oriented single-walled CNT (SWCNT) arrays. Indeed, the ability to prepare vertically aligned SWCNTs is a crucial point for improving the performance of nanodevices. [9] Covalent attachment of vertically aligned SWCNTs is usually achieved by amide linkages. [10] Recently, we reported the formation of dense arrays of SWCNT "forests" on different substrates by using diazonium salt coupling. [11] Nevertheless, a valid alternative is represented by the noncovalent direct immobilization of SWCNTs on a surface, since in this case no structural alteration of the SWCNTs occurred. [12] In view of the growing interest in the construction of simple and cost-effective systems, we report herein a new strategy to achieve a spatially controlled SWCNT assembly on a gold surface by exploiting p-p interactions. To the best of our knowledge, no report on the oriented and reversible assembly of SWCNTs on a surface by using noncovalent p-p stacking interactions has been reported to date. In particular, the proposed method is based on the spontaneous adsorption of SWCNTs on self-assembled monolayers (SAMs) of suitable aromatic molecules. To this end, a stable dispersion of purified SWCNTs (HiPCO) in DMF was obtained by sonication, as previously described. [13] The average length of the suspended SWCNTs was 60-120 nm, as evaluated by transmission electron microscopy (TEM).The adsorption of SWCNTs was achieved by immersing Au surfaces that were modified with SAMs of phenylthiol (PT), 4,4'-dithiobipyridine (DTBPY), and biphenylthiol (BPT) overnight in a suspension of SWCNTs. The adsorption kinetics were investigated by using a quartz crystal microbalance (QCM). The frequency changes (Df) of the Au/quartz crystal modified with different SAMs increased upon the immobilization of SWCNTs ( Figure S1 in the Supporting Information). After the adsorption was complete (ca. 90 min), we estimated that approximately 3.4 AE 0.2 (Df = À572 Hz), 3.9 AE 0.1 (Df = À658 Hz), and 6.7 AE 0.2 (Df = À1125 Hz) mg cm À2 of SWCNTs were present on the surface modified with PT, DTBPY, and...