We synthesized and investigated ultrafast third-order optical response of iron(III) (Fe(III)) and ruthenium(III) (Ru(III)) coordinated fullerene derivatives, which were based on our former reported C-60(NH2CN)(5) series, at 830 nm. The Fe(III), which is electron deficient and blocks the intramolecular charge-transfer process, reduces the optical nonlinearity of the complexes. However. Ru(III), even it is also electron deficient, enhanced the optical nonlinearity for an order of magnitude. By analyzing the infrared spectrum, a possible effect of linked multi-fullerene molecule system is supposed.