1,2-Migration of ligands across metal-metal bonds is an increasingly common phenomenon in the study of heterometallic complexes. For example, Lu and coworkers have reported the 1,2-migration of a mesityl group between Ni and Al sites that could be induced by the coordination of different donor ligands. Okuda, Maron and coworkers described a heterometallic Zn-Ga system, in which a hydride ligand reversibly migrates between the two metals, with the position of the equilibrium determined by solvent. Examples of double 1,2-migration of two ligands from one metal to the other are considerably rarer. Perhaps the best characterised example is a simultaneous transfer of two hydride ligands from a Ga to a Rh centre documented by Aldridge and coworkers. Through isolation and crystallographic characterisation of a series of Ga-Rh complexes, snapshots of the reaction coordinate of the double ligand migration could be obtained. We have suggested that this double 1,2-migration event is an important step in the C-H functionalisation of arenes catalysed by Pd-Al heterometallic complexes. Dyotropic rearrangements at heterometallic complexes are rarer still. To the best of our knowledge precedent is limited to one well-defined example; Braunstein, Knorr, Hoffmann and coworkers reported a Fe-Pt system, where ligand exchange can induce a simultaneous transfer of a silyl ligand from Fe to Pt and that of carbonyl or isocyanide from Pt to Fe. There is a parallel between this system and known rearrangements of first row transition metal carbonyl dimers. These species can undergo degenerate dyotropic rearrangements with exchange of CO between the two metal centres. In this paper, we report the exchange of hydride and carbonyl ligands in a heterometallic Fe-Al complex by a dyotropic rearrangement. Computational analysis suggests that the reaction is initiated by the coordination of the CO ligand to Al, followed by migration of the hydride to Al and carbonyl to Fe. The change in coordination environment fundamentally changes the electronics and the reactivity of the heterometallic complex -switching its properties and exposing new reactivity of hydridic sites that previously did not exist.