Two-electron reduction of [(eta5-C5H4Me)4Fe4(mu3-CH)2(mu3-CO)2](PF6)2 (1) results in the coupling of two methylidyne ligands to form (eta5-C5H4Me)4Fe4(HCCH)(mu3-CO)2 (2), the two-electron oxidation of which reproduces 1. Structures of 1 and 2 were determined by X-ray diffraction analysis.