Charged (macro)molecules are essential components in natural materials and organisms; thus the rational design of biomimetic materials requires a holistic understanding of structure–property relationships in charged systems. We discuss recent progress in uncovering such relationships for polyzwitterions and polyelectrolyte complexes, with emphases on the synthetic strategies that were employed in systematic studies. For polyelectrolytes, discussion is confined to the effects that structural variations in polycation and polyanion structure have on the fundamental phase behavior of the corresponding polyelectrolyte complexes. In the field of polyzwitterions, both fundamental and applied properties are discussed in relation to chemical structure. Finally, we present an overview of promising chemistries that will expand the structural landscape of charged macromolecules with the aim of stimulating new research to further uncover and understand the fundamental design principles for these materials.

带电（大分子）是天然物质和有机体中必不可少的成分。因此，仿生材料的合理设计要求对带电系统中结构与属性之间的关系有一个整体的了解。我们讨论了揭示两性离子和聚电解质络合物的这种关系的最新进展，重点是系统研究中采用的合成策略。对于聚电解质，讨论仅限于聚阳离子和聚阴离子结构中的结构变化对相应的聚电解质配合物的基本相行为的影响。在多性两性离子领域，讨论了与化学结构有关的基本性质和应用性质。最后，