In the nanoimprint process, the resolution limit of patterning has attracted much attention from both scientific and industrial aspects. In this article, we briefly review the main achievements of our research group on subnanoscale nanoimprint fabrication of atomically patterned glassy substrates of oxide glass and polymer. By applying the sapphire (a-Al 2 O 3 single crystal) wafers with self-organized nanopatterns of atomic steps as thermal nanoimprinting molds, we successfully transferred their nanoscale patterns onto the surfaces of glassy substrates such as sodalime silicate glasses and poly(methyl methacrylate) polymers. The surfaces of nanoimprinted glassy materials exhibited regularly arrayed atomic stairs with 0.2-0.3 nm step height, which were in good agreement with the subnanopatterns of sapphire molds. These atomically stepped morphologies on the glassy substrates were found to be stable for about 1 year.