The selective capture of heavy metal ions is a major challenge due to the need for materials with high affinity, selectivity, and capacity. Nature uses proteins to manage metal ions via specific structural motifs. This focus review summarizes recent advances in bioinspired and biosynthetic integrated strategies for the capture of heavy metal ions. The topics discussed include (1) the structural and thermodynamic features of metal-binding proteins, (2) synthetic polymers that mimic the biological functions of proteins, and (3) hybrid materials that integrate biological (macro)molecules with synthetic polymers.