The synthesis and characterization of the cationic mixed metal Ga/Zn cluster [Zn-2(GaCp*)(6)](2+) (1) is presented. The reaction of [Zn2Cp*(2)] with [Ga2Cp*][BAr4F] leads to the formation of the novel complex being the first example of a [Zn-2](2+) core exclusively ligated by metalloid group-13 organyl-ligands. Compound 1 exhibits two different coordination modes: In the solid state, two of the six GaCp* ligands occupy bridging positions, whereas VT H-1 NMR indicates the coexistence of a second isomer in solution featuring six terminal GaCp* ligands. Quantum chemical calculations have been carried out to assign the gallium and zinc positions; the bonding situation in 1 is characterized and the importance of dispersion forces is discussed.