Herein we present the first double deprotonation of acetonitrile (CH3CN) using 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 is primarily ionic in nature. Mechanistic studies reveal the intermediacy of a monomeric [CH2CN]– complex, which has been characterised in-situ. Our findings provide an important example in which a bimetallic metal complex achieves a new type of reactivity not previously encountered with monometallic counterparts. The isolation of a [CHCN]2– dianion through simple deprotonation of CH3CN also offers the possibility of a establishing a broader chemistry of this motif.