One of the recent strategies being explored for obtaining molecular magnets with enhanced properties is the incorporation of heavier transition metals from the 4d and 5d metal ions. [1][2][3] A central player in this area of research is the cyanide ligand, which can be used to prepare mixed metal clusters with unusual properties. [4] Of particular interest is the fact that cyanide molecules containing 4d or 5d ions or combinations of them with 3d ions have been predicted to behave as singlemolecule magnets (SMMs) with higher blocking temperatures T B than those based on 3d ions. They are also expected to exhibit properties such as anisotropic magnetic exchange interactions. [5] A main driving force for the high activity in cyanide magnetism is that the use of cyanometalates in reactions with metal ions equipped with capping ligands present several advantages, such as control over the sign of magnetic interactions in most cases and also predictable structures based on the building block approach. Magnetic anisotropy can be conveniently introduced by choosing the appropriate preformed 4d or 5d cyanometalate anion. The observation of SMM behavior with 4d and 5d metal ions with oxygen-type bridging ligands is limited to only one case, [6] but there are a number of SMMs from the heavier congeners of Groups 6 and 7 with the precursors [(Me 3 tacn)Mo III (CN) 3 ], [7] [Mo V (CN) 8 ] 3À , [8,9] [W V (CN) 8 ] 3À , [8][9][10] [Re IV (CN) 7 ] 3À , [11] and [(triphos)Re II (CN) 3 ] À . [12] In contrast to the widely investigated anion [Mo V (CN) 8 ] 3À , [2,8,9] the heptacyanomolybdate derivative [Mo III (CN) 7 ] 4À has received much less attention in the molecular magnetism field, presumably because of the synthetic challenges in the preparation and handling of this anion. Unlike the hexa-and octacyanometalates, the [Mo III (CN) 7 ] 4À anion favors low-symmetry extended structures with pronounced magnetic anisotropy. [1,13] The results of theoretical investigations have suggested that [Mo(CN) 7 ] 4À will be useful for the design of SMMs with high T B values as a result of its strong anisotropic exchange properties. [5] Despite such promising predictions, magnetic materials based on [Mo(CN) 7 ] 4À are relatively scarce, with the exception of the pioneering work of Kahn and co-workers, and subsequent studies by several other research groups, who prepared a number of two-and three-dimensional magnets with the [Mo(CN) 7 ] 4À and Mn II ions. [1,13] The only other reports are an amorphous compound with iron(II) [14] and two microcrystalline materials with vanadium(II) and nickel(II). [15] To our knowledge, no discrete clusters based on [Mo(CN) 7 ] 4À have been reported.Given the aforementioned considerations, we recently devoted efforts to the preparation of mixed-metal molecules that contain the [Mo(CN) 7 ] 4À building block. Herein, we report the first discrete compound based on [Mo(CN) 7 ] 4À