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In order to gain a deeper insight into structure-property relationships of the donor (D)−acceptor (A) interactions in cationic sesquifulvalene complexes the mono-and dicationic complexes [(η 5 -C 5 H 5 )Fe{µ-(η 5 -C 5 H 4 )(η 7 -C 7 H 6 )}MЈLЈ] + were synthesized as BF 4 and PF 6 salts: MЈLЈ = Cr(CO) 3 (3PF 6 ); MЈLЈ = none (4BF 4 ); MЈLЈ = Ru(η 5 -C 5 H 5 ) + [5(PF 6 ) 2 ]; MЈLЈ = Ru(η 5 -C 5 Me 5 ) + [6(PF 6 ) 2 ]. The ferrocenyl substituent works as the electron donor and the tropylium moiety as the electron acceptor. For the electronic ground state the NMR spectroscopic results demonstrate an increasing charge delocalization in the order MЈLЈ = Cr(CO) 3 Ͻ Ru(η 5 -C 5 Me 5 ) + Ͻ Ru(η 5 -C 5 H 5 ) Ͻ none. The same order of the acceptor moieties is observed for the difference between the oxidation and reduction potentials, which are related to an electrochemically reversible and a complete irreversible one-electron transfer, re- [a]