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(Cyclopentadienone)iron carbonyl complexes have recently received particular attention for their use as catalysts in hydrogenation or transfer hydrogenation reactions including the N-alkylation of amines with alcohols. This is due to their easy synthesis from simple and cheap materials, air and water stabilities, and the crucial metal–ligand cooperation giving rise to unique catalytic properties. Here, we report a Mössbauer spectroscopic and computational investigation of such a complex and its corresponding activated species for dehydrogenation and hydrogenation reactions. This study affords a deeper understanding of the species formed by the reaction with Me3NO and their distribution upon the added amount of an oxidant.