hydrogen bonds · magnetic properties · metalorganic frameworks · multiferroic compounds · solid-state structuresThe realization of ever smaller tunable devices is a major challenge in nanoelectronics; as a result, considerable efforts have been devoted to multifunctional materials in the last few years. Multiferroic compounds in which magnetic and electric properties coexist have received much attention. The observation of combined weak ferromagnetism and antiferroelectric order in a metal-organic framework (MOF) from Jain et al. illustrates a new route towards multiferroic systems that significantly differs from usually reported studies. [1] Multiferroic materials present at least two coexisting orders among the electric, magnetic and/or elastic ones. The most appealing combination to date involves electric and magnetic orders, as it opens great perspectives in terms of applications, especially in the field of spintronics.[2] A clear distinction has to be made between systems exhibiting independent electric and magnetic orders and those featuring a magneto-electric coupling, both of which are promising in terms of applications. The former allows, for example, the conception of a four-state memory, [3] but the greatest promise is likely to be held by magneto-electric compounds, for they give access to a new type of control of magnetization by an electric field in spintronics devices. [4] The heart of the problem currently is to find examples of multiferroic/magnetoelectric materials. One option is, of course, to combine the properties of two separate materials, one being ferromagnetic, the other ferroelectric, in a nanostructured composite material.[5] The coupling between both, which allows their mutual control, is usually carried out indirectly through strain by magneto-and electro-striction, which results in slow switching and fatigue phenomena. Intrinsic multiferroics are thus highly desirable, although, as mentioned by Jain et al., electric and magnetic orders tend to be mutually exclusive. Indeed, the presence of d electrons of transition metal ions, which are required to stabilize ferromagnetism, inhibits hybridization with the p orbitals of the surrounding oxygen anions, and thus displacement of the cations necessary for the establishment of a ferroelectric order. [6] Intrinsic multiferroic materials, which are scarce, are generally classified according to the mechanism responsible for ferroelectricity: in proper ferroelectrics, spontaneous polarization appears as being itself the order parameter, whereas in improper ferroelectrics, it only appears as a by product in a phase transition governed by another order parameter. [7] For the former, the magnetic and electric orders are usually due to distinct cations, and the magnetoelectric coupling is generally weak. The prototypical compound is BiFeO 3 (BFO), in which 3d electrons of the iron(III) cations are responsible for magnetization, whereas ferroelectricity originates from a structural instability caused by the hybridization between the oxygen 2p and th...