A new group of CO-releasing molecules, CO-RMs, based on cyclopentadienyl iron carbonyls have been identified. X-Ray structures have been determined for [(η-C5H4CO2Me)Fe(CO)2X], X = Cl, Br, I, NO3, CO2Me, [(η-C5H4CO2Me)Fe(CO)2]2, [(η-C5H4CO2CH2CH2OH)Fe(CO)2]2 and [(η-C5H4CO2Me)Fe(CO)3][FeCl4]. Half-lives for CO release, 1H, 13C, and 17OC NMR and IR spectra have been determined along with some biological data for these compounds, [(η-C5H4CO2CH2CH2OH)Fe(CO)3]+ and [{η-C5H4(CH2)nCO2Me}Fe(CO)3]+, n = 1, 2. More specifically, cytotoxicity assays and inhibition of nitrite formation in stimulated RAW264.7 macrophages are reported for most of the compounds analyzed. [(η-C5H5)Fe(CO)2X], X = Cl, Br, I, were also examined for comparison. Correlations between the half-lives for CO release and spectroscopic parameters are found within each group of compounds, but not between the groups.