Existing examples of Peierls-type 1D systems on surfaces involve depositing metallic overlayers on semiconducting substrates, in particular, at step edges. Here we propose a new class of Peierls system on the ð1010Þ surface of metal-anion wurtzite semiconductors. When the anions are bonded to hydrogen or lithium atoms, we obtain rows of threefold coordinated metal atoms that act as one-atom-wide metallic structures. First-principles calculations show that the surface is metallic, and below a certain critical temperature the surface will condense to a semiconducting state. The idea of surface scaffolding is introduced in which the rows are constrained to move along simple up-down and/or sideways displacements, mirroring the paradigm envisioned in Peierls's description. We predict that this type of insulating state should be visible in the partially hydrogenated ð1010Þ surface of many wurtzite compounds. DOI: 10.1103/PhysRevLett.117.116101 The electronic, vibrational, and magnetic properties of 1D systems are central to current condensed matter physics, from Luttinger liquids to nanotubes and nanowires. Part of the driving force behind this interest is linked to unique properties that 1D systems offer, which may be exploited in nanoscaled electronic and sensing devices. Metallic chains in one dimension, however, are generally unstable and undergo a metal-insulator (MI) phase transition at low temperatures-the so-called Peierls instability [1,2]. In the classical Peierls picture, the MI transformation is driven by electronic redistribution via the opening of a band gap at the Fermi level. The Fermi surface nesting features of the original unit cell cause the electronic instability and, consequently, a reduction in total energy. The electronic redistribution of filled states near the Fermi level sets up a charge density wave (CDW) [3-6] responsible for a metal-toinsulator transition. Although the main driving force in a Peierls transition is electronic, the MI transition in real systems is always accompanied by a periodic lattice distortion resulting in a new unit cell due to the strong chargelattice coupling.CDW in low-dimensional systems deposited on substrates have been reported [7] for quasi-2D systems such as submonolayers of Pb=Sn Ge(111) [8][9][10] and In=Cuð001Þ [11], and quasi-1D systems such as bands of In=Sið111Þ [12][13][14][15][16][17], Au=Geð001Þ [18,19], and Au=Sið553Þ [20,21]. In the quasi-1D systems studied so far, the width (w) of each metal band was at least four to five atoms across. However, later studies on these quasi-2D and -1D systems have called attention to the fact that more complex structural reconstruction forces unrelated to the Peierls transition may be present for all of these cases [22,23]. Indeed, detailed mapping of the Fermi surfaces [24] have revealed a behavior that does not meet the Peierls transition criterion. Effects of atoms from deeper layers are found to be strong on the seemingly 1D systems [25][26][27]. Further, it has proven very difficult to fabricate, by direct d...