A distinguishing feature of molecular-based magnetic materials is that the vast majority of examples are insulators, and the microscopic magnetic moments are therefore localised. Maximum connectivity between centres carrying the moments is therefore desirable to maximise ordering temperatures, so ambidentate ligands are most effective. We have been studying the bimetallic tris-oxalato series AMFe(III)(C2O4)(3) from this point of view and the lecture will give an overview of results. We concentrate on organic cations A stabilising a hexagonal layer structure since the details of magnetic ordering are highly sensitive to changes in the packing of A between the layers. In contrast when A = BEDT-TTF the organic layer is conducting and in one case superconductivity has been found.