Knowledge and control of the self-organization of materials are the essential foundations not only for understanding the mechanism of the phenomenon but also for the development of functional materials and devices for practical applications. In fact, among the recent developments in nanoscale science and technology, the realization of new functions via self-organization is the basis of many brilliant innovations and is one of the main goals of researchers. Efficient use of the multifold characteristics of organic materials plays important roles. [1][2][3][4][5][6][7][8][9][10][11][12] The formation of nanostructures is achieved, in general, by controlling the direct and indirect interactions between building blocks, originating from, for example, electronic and conformational structures, strains, and chemical reactions. Recently, a selective supramolecular assembly of adsorbed molecules, for example, has been successfully produced through the chemical modification of functional groups. 1 For the further advance of the nanostructurebased functional devices, the understanding and control of the electronic properties of self-organized structures based on such a modification of interactions are key factors for success.Here, we demonstrate a two-dimensional (2D) anisotropic electronic structure produced through the formation of a selfassembled monolayer (SAM) of glycine molecules on a Cu(100) surface. A standing wave originating from the 2D electronic structure was visualized, for the first time, for the SAM of organic molecules, and the anisotropic dispersion relations reflecting the structure of the SAM were obtained.Glycine is the simplest amino acid and does not have any active functional groups except for the carboxyl and amino groups, which are common to all amino acids, and one of the fundamental components of biological molecules such as proteins and peptides. Glycine molecules are evaporated in a neutral form (NH 2 CH 2 -COOH). When the substrate is maintained at room temperature (RT), the hydrogen atom in the carboxyl group is removed from the surface and glycine molecules are adsorbed in a glycinate form (NH 2 CH 2 COO -). 12,13 The two oxygen atoms in the carboxylate group and the nitrogen atom in the amino group, which are located on the top sites of Cu(100), are bonded to the Cu atoms, where the carboxyl and amino groups are negatively and positively polarized, respectively. Among the amino acids, glycine is the only molecule that does not have chirality, but enantiomeric isomers are observed on the Cu surface depending on the directional relationship of the two groups in the adsorbed form, as schematically shown in Figure 1c. The adsorption properties of this system are well characterized, indicating the importance of this material for understanding and application of the basic mechanism of the self-organization of a polarized molecule with chirality.In addition to sample preparation, scanning tunneling microscopy and spectroscopy (STM/STS) measurements were performed under ultrahigh vacuum conditions ...