Recent advances in the fields of liquid crystals and supramolecular chemistry have led to the discovery of mesomorphic metallo-helicates formed by selective complexation of non-mesomorphic oligopyridinic ligands built from flexible imino-appendages. Different types of mesophases, ranging from columnar to ordered smectic biaxial, have been generated. In cases where the segmented ligand is adequately engineered, gliding of the coordinated ligands across the metal centers present in the emergent dinuclear complex is made possible by the provision of ancillary imino binding sites and this behavior facilitates liquid-crystalline proper-ties at room-temperature, after supercooling. Furthermore, formation of a mesogenic mixed-valence complex following selective oxidation has been realized. An attempt is made to provide insight on how the strategy of using imino-based oligopyridinic scaffolds pen-nits generation of liquid-crystalline materials with morphologies determined by their molecular components.