This chapter sketches an outline of ferrocene–peptide bioconjugates. A variety of ferrocene–peptide bioconjugates have been designed to induce highly ordered structures of peptides and develop new biomaterials. The ferrocene serves as a reliable organometallic scaffold for the construction of an ordered structure via intramolecular hydrogen bonding, wherein the attached peptide strands are regulated in appropriate dimensions. Another noteworthy feature of ferrocene–peptide bioconjugates is their strong tendency to self-assemble through the contribution of available hydrogen bonding sites in the solid state. Furthermore, the ferrocene moiety of ferrocene–peptide bioconjugates is able to act as a redox-switching center and an electrophore in the receptors and biomaterials.