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Herein we present the first double deprotonation of acetonitrile (CH3CN) using two equivalents of a bimetallic iron‐aluminium complex. The products of this reaction contain an exceeding simple yet rare [CHCN]2− dianion moiety that bridges two metal fragments. DFT calculations suggest that the bonding to the metal centres occurs through heavily polarised covalent interactions. Mechanistic studies reveal...