AbstractStructure‐resonance theory can be used to derive charge distributions and bond orders in ferrocenes, open ferrocenes and α‐ferrocenylalkyl cations. These species are of interest because they are unusually accessible and stable and understanding the electronic origin of this stabilization would aid in developing bonding models for organometallic systems. The methods for carrying out the calculations will be outlined. They involve shortcuts and algorithms for counting structures. The choice of structure basis, limited to conventional principal resonance structures, will be discussed. Charges and bond orders will be compared with NMR chemical shift and X‐ray data. The unusual stabilities of the ions and the role of the metal in stabilizing positive charge will be understandable within the conventional ideas of structural organic chemistry and resonance theory. These metal‐organic systems are highly delocalized and consequently resonance stabilized to a significant degree. They can be characterized as three‐dimensional aromatic