New ditopic bis-hydrazone type ligands possessing various functional units have been designed to self-assemble into axially and laterally decorated [2 x 2] grids with octahedrally coordinating metal ions. Solution and solid state investigations have provided evidence for the strong influence of the nature of the attached groups on the structure and function of these metallo-supramolecular entities. Various techniques were applied in order to explore the magnetic, optical and structural properties of these functional nanosize platforms. The results obtained showed the effect of ligand functionalization both on the ease of formation of the grid architectures and on their physicochemical properties.