Abstract: The progress of the research on material selection and structure design for superhard nano-multilayer films is summarized.The material selection for the multilayer films is mainly introduced.The factors in realizing the superhard characteristics of multilayer films needed to be considered are summarized from several aspects including the material types used for multilayer films,the selection of film and substrate,material selection and the inspiration obtained from the superhard effect theory. The current problems and development are pointed out.