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The reaction of [Cp 2 Mo 2 (CO) 4 (μ,η 2:2 ‐E 2 )] ( A : E=P,  B : E=As, Cp=C 5 H 5 ) with the WCA‐containing Cu I  salts ([Cu(CH 3 CN) 4 ][Al{OC(CF 3 ) 3 } 4 ] (CuTEF,  C ), [Cu(CH 3 CN) 4 ][BF 4 ] ( D ) and [Cu(CH 3 CN) 3.5 ][FAl{OC 6 F 10 (C 6 F 5 )} 3 ] (CuFAl,  E )) affords seven unprecedented coordination compounds. Depending on the E 2  ligand complex, the counter anion of the copper salt and the stoichiometry, four dinuclear copper dimers and three trinuclear copper compounds are accessible. The latter complexes reveal first linear Cu 3  arrays linked by E 2  units (E=P, As) coordinated in an η 2:1:1  coordination mode. All compounds were characterized by X‐ray crystallography, NMR and IR spectroscopy, mass spectrometry and elemental analysis. To define the nature of the Cu⋅⋅⋅Cu⋅⋅⋅Cu interactions, DFT calculations were performed.

Linking of Cu I Units by Tetrahedral Mo 2 E 2 Complexes (E=P, As)