Bio-related science has been one of the most important fields in the viewpoint of health and welfare of human being. A biofunctionalization of inorganic nanoparticles becomes more and more important in the near future, since it allows what is called theranostics, a new concept of next-generation medicine that combines therapeutics and diagnosis. Ever since the notion of intercalative bioinorganic nanohybrids was created based on the layered double hydroxide (LDH) material, a variety of bio-LDH nanohybrids have been developed to provide new opportunities toward theranostic biomedical applications. In this chapter, we review the structural chemistry of several bio-LDH nanohybrids available for gene and drug delivery system and focus on the platform strategies for advanced theranostic system. The cellular trafficking mechanism of LDH and cancer therapeutic efficacy along with diagnostic imaging of the bio-LDH nanohybrids are also discussed in in vitro as well as in vivo studies.