Inorganic macrocycles based on P(III)–N bonded frameworks can be obtained by a series of systematic routes, many of which parallel those commonly employed in the synthesis of more well known organic relatives. Such phosph(III)azane macrocycles exhibit a broad range of coordination behaviour, and provide new organically-soluble hosts, with unique steric and electronic environments. This short review explores designed approaches to this class of macromolecule and the coordination of anionic, cationic and neutral guests, and looks to the future development of related inorganic systems of this type.