Since the middle of the 20th century, metallopolymers have represented a standalone subfield with a beneficial combination of functionality from inorganic metal centers and processability from the organic polymeric frameworks. Metallo-polyelectrolytes are a new class of soft materials that showcase fundamentally different properties from neutral polymers due to their intrinsically ionic behaviors. This review describes recent trends in metallo-polyelectrolytes and discusses emerging properties and challenges, as well as future directions from a perspective of macromolecular architectures. The correlations between macromolecular architectures and properties are discussed from copolymer self-assembly, metallo-enzymes for biomedical applications, metallo-peptides for catalysis, crosslinked networks, and metallogels.