Dedicated to Professor The Lord Lewis on the occasion of his 75th birthdayHigh-nuclearity mixed-metal clusters have aroused considerable attention because of their ability to act as an ™electron reservoir∫, the potential to precisely control the ratio and geometry of the two metals involved, [1] and their potential application in catalysis.[2] Reactions of cluster anions with palladium±halide complexes were found to be effective in producing high-nuclearity mixed-metal clusters, for example, [Fe 6 Pd 6 (CO) 24 H] 3À , [3] [Ru 10 Pd 8 C 2 (CO) 27 (C 3 H 5 ) 4 ], [4] and [Ni 9 Pd 33 (PPh 3 ) 6 (CO) 41 ]À .[5]However, high-nuclearity osmium±palladium mixed-metal clusters prepared by a similar approach are rare.[6] We recently established a reliable route to preparing such species in moderate yield using a decaosmium cluster anion and a palladium cation as the starting materials. Herein, we report the synthesis and structural characterization of the novel high-nuclearity sandwich osmium±palladium mixed-metal cluster [{N(PPh 3 ) 2 } 2 {Os 18 Pd 3 -(m 6 -C) 2 (CO) 42 þ salt (1) in 37 % yield. An insoluble black solid was also obtained from the reaction mixture; IR spectroscopy indicated that the solid material may consist of highnuclearity carbonyl±metal clusters.Single crystals of 1 suitable for X-ray analysis were obtained as dark-green blocks by slow evaporation of the CH 2 Cl 2 /MeOH solution mixture at 0 8C. The molecular structure, together with some important bond parameters, is depicted in Figure 1. The structure of 1 can be described as a giant dumbbell-shaped bimetallic nanocluster. The cluster core-geometry can be divided into three metallic domains. A triangular Pd 3 metal unit is sandwiched between two tricapped octahedral {Os 9 (m 6 -C)(CO) 21 } subclusters, which combine to give an overall D 3h symmetry. The five ABABA closepacked layers of metal ions (6:3:3:3:6) that are shown in Figure 2 are unprecedented in existing Os±Pd mixed-metal clusters. The central {Os 3 Pd 3 Os 3 } unit, which consists of the Os7, Os8, Os9, Pd1, Pd2, Pd3, Os10, Os11, and Os12 metal ions, forms a face-sharing bioctahedron that is reminiscent of the Rh 9 geometry observed in the [Rh 9 (CO) 19 ] 3À ion.[9] The palladium ions, which form the edge-sharing face of the bioctahedron only possess metal±metal bonding character; there are no bonds to carbonyl ligands, which is very unusual. This naked metal triangle is relatively exposed, which may facilitate the coordination of nucleophiles. For the two osmium domains, two Os 9 units are in an eclipsed conformation, which is contrary to the closely related osmium±mercury mixed-metal cluster, [{N(PPh 3 ) 2 } 2 {Os 18 Hg 3 (m 6 -C) 2 (CO) 42 }].