SummaryUltraflat surface substrates are required to achieve an optimal performance of future optical, electronic, or optoelectronic devices for various applications, because such surfaces reduce the scattering loss of photons, electrons, or both at the surfaces and interfaces. In this paper, we review recent progress toward the realization of ultraflat materials surfaces. First, we review the development of surface-flattening techniques. Second, we briefly review the dressed photon–phonon (DPP), a nanometric quasiparticle that describes the coupled state of a photon, an electron, and a multimode-coherent phonon. Then, we review several recent developments based on DPP-photochemical etching and desorption processes, which have resulted in angstrom-scale flat surfaces. To confirm that the superior flatness of these surfaces that originated from the DPP process, we also review a simplified mathematical model that describes the scale-dependent effects of optical near-fields. Finally, we present the future outlook for these technologies.