Mechanistic studies suggest that the product is formed via a [CH2CN] -monoanion intermediate. This species could be spectroscopically characterised in-situ. DFT calculations suggest that the unique reactivity can be conceptualised in terms of two successive deprotonation steps, both of which are driven by the high basicity and unusual properties of the Fe-Al bimetallic complex. Our findings open up the possibility of a wider chemistry of simple [CHCN] 2-dianions including potential applications as chemical building blocks for synthesis.