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Reduction of the Ir4(CO)12 cluster by two equivalents of Cp*2Cr (Cp* is η5‐Me5C5) produces the (Cp*2Cr+)2{Ir4(CO)11−}2 ⋅ 4 C6H4Cl2 complex. Two Ir4(CO)11− anions are bonded by a single Ir−Ir bond in the anionic {Ir4(CO)11−}2 dimer. The bond length is 2.8339(5) Å at 100 K. Therefore, clusters can form metal‐metal bonded dimers under reduction. The {Ir4(CO)11−}2 dimers do not dissociate to paramagnetic...