The widespread interest in the use of biomimetic approaches for inorganic nanomaterial synthesis have led to the development of biomolecules (peptides, nucleic acids) as key components in material synthesis. Using biomolecules as building blocks, additional functionalities can be introduced by engineering multifunctional peptides that are capable of binding, nucleating, and assembling multiple materials at the nanoscale. We describe methodologies that exploit peptides for the synthesis of bimorphic nanostructures.