© 2020 The Chemical Society of Japan Several fabrication technologies for molecular level ultra-thin films, from organic to organicinorganic hybrids, are introduced using the surface imaging technology of scanning probe microscopy (SPM). Electrochemical scanning tunneling microscopy (EC-STM), atomic force microscopy (AFM) and related techniques enable the observation of the surface of 2D materials in near real-time and in real-space. The combination of 2D materials and SPM technology opens up a new avenue of surface and material science, despite its many restrictions.