CASSCF calculated wavefunctions are presented for three f-element metallocenes, MCOT2 (M = Ce, Th, Pu; COT = η(8)-C8H8). The configurational admixture of these systems is investigated and, where the ThCOT2 ground state is well-defined as a monodeterminantal Th(iv) state, the cerocene ground state is found to be strong multiconfigurational and to bear strong similarities to that of plutonocene. Associated electronic densities are studied using QTAIM topological analysis and compared to CASSCF-derived densities of the aromatic systems benzene and the COT dianion. This analysis provides evidence of enhanced covalent character in plutonocene, supporting structural data calculated previously. Evidence of charge localisation in found in cerocene, this being most pronounced in its excited state of Ag symmetry. QTAIM analysis reveals that the ligand electronic structure is very similar in all metallocenes, and density differences show little variation in the ligand between the cerocene ground and excited state. Orbital contributions to integrated QTAIM properties are considered, and excellent agreement with experimentally determined f-orbital occupation is obtained. All methods of analysis support a Ce(iv) or mixed valence assignment of the cerocene ground state, whereas the Ag excited state is best described as a Ce(iii) state.