A number of biological systems have developed highly orchestrated detoxification mechanisms toward the bioreduction and mineralization of noble metals. These systems incorporate small peptides and proteins as nucleation sites for metal binding and nanocluster stabilization. Herein, we present the use of biologically relevant ligands ranging from single amino acids (histidine, imidazole, and cysteine) to linear peptides (glutathione and a histidine rich peptide) in the stabilization of a variety of noble metal surfaces (Au-0, Ag-0, Pt-0, and Cu-0). As a result, the different nanocluster/ligand combinations offered a broad range of sizes and stabilitites. The peptide coat also affords a unique functional handle for the formation of larger assemblies. Using Ni chelation and immunomolecular approaches, strategies for the assembly of nanocluster heterostructures were investigated.