Negatively charged amino acids (aspartic acid, glutamic acid) and a related polymer, poly(alpha,beta-aspartate),have been intercalated within the gallery spaces of layered double hydroxides. Synthesis of these bioinorganic nanocomposites was achieved via coprecipitation involving simultaneous formation of the inorganic layers and intercalation of the anionic species. In situ thermal polymerization of pre-intercalated aspartate monomers affords a second route to the poIy(alpha,beta-aspartate)-containing hybrid material.