The first complex with an M(3)Te(7) cluster core, [Mo-3(mu(3)-Te)(mu(2)-Te-2)(3)(CN)(6)](2-), has been synthesized by the extrusion reaction of the solid-state product of the high-temperature reaction of molybdenum, tellurium, and iodine with aqueous cyanide. Short Te...I contacts play an important role in the crystal packing of the title compound and lead to the formation of quasi-two-dimensional layers. Reactivity of tellurium-rich Mo3Te7 cluster complexes in chalcogen-transfer reactions is drastically different from that of sulfide and selenide analogs.