IntroductionOver the past few years there has been considerable interest in nanoscale materials which often exhibit unique physical and chemical properties that are dramatically different from their bulk counterparts.1–3More recently, nanohybrids, defined as composites consisting of two disparate nanoscale materials with two different functions,e.g.a mixed conductor consisting of an electronic conducting phase and ionic conducting one,4which are chemically bound in an organized way. Such materials often exhibit extraordinarily high synergetic and complementary behavior.In particular, the combination of two-dimensional layered materials and the intercalation technique offers new areas for developing new hybrids with desired functionality.5–14Since most biomolecules, such as nucleoside monophosphates and ATP are negatively charged, they can be incorporated between the hydroxide layers as the charge compensating anions through ion exchange.15,16Layered double hydroxides (LDHs), also called ‘anionic clays’, have received considerable attention due to their technological importance in catalysis, separation technology, optics, medical science, and nanocomposite materials engineering. LDHs consist of positively charged metal hydroxide layers, in which the anions (along with water) are stabilized in order to compensate the positive layer charges. The composition can be generally represented as [M2+1 − xM3+x(OH)2][An−]x/n·mH2O,where M2+is a divalent cation (Mg2+, Ni2+, Cu2+, and Zn2+), M3+is a trivalent one (Al3+, Cr3+, Fe3+, V3+, and Ga3+), and Ax/nn−is an anion with chargen. Various kinds of inorganic or organic anions (An−) have been introduced between the hydroxide layers by simple ion-exchange reaction or coprecipitation.17–20Especially, LDHs consisting of magnesium and aluminium have already been used as antiacid and antipepsin agents, therefore, we believe that the present LDH is quite bio-compatible. In the present study, novel bio-hybrids of layered double hydroxide (LDH) and biomolecules (ATP or nucleoside monophosphates) aredesigned and organized artificially on the nanometer scale to provide opportunities for reservoir and delivery carriers of functional biomolecules in gene therapy and drug delivery. Therefore, the purpose of this study is not only to prepare new bio-inorganic nanohybrids but also to provide basic data for developing new inorganic carriers.