Metal ions play crucial roles in mediating the structures and functions of metalloproteins in biological systems. This review summarized the progress of using rational design of artificial metal-binding sites to expand the functional diversity of proteins, which includes designing artificial metal-binding sites within protein scaffolds by exploring potential metal-binding sites, redesigning existing metal-binding sites, or designing new metal-binding sites, and on the protein surfaces to achieve structural and functional conversions, studying interactions with nanomaterials, or performing prot...