The very first examples of protein/DNA/inorganic nanocomposite materials are described. Surprisingly, the presence of DNA enhanced the properties of the bound protein. The layered inorganic solid, alpha-Zr(IV) phosphate (alpha-Zr(HPO4)2.H2O, abbreviated as alpha-ZrP) served as an excellent host for these studies, and the binding has been carried out under benign conditions (aqueous solutions at room temperature and neutral pH). These novel nanobiocomposite materials provide a simple method for the binding of DNA to negatively charged solids, and such approaches aid in engineering more effective synthetic materials for gene-delivery, RNA-delivery and drug delivery applications.