Two homochiral trinuclear clusters, {(MeTP)(2)Fe-2(CN)(6)Ni[(1R,2R)-chxn](2)} (1) and {(MeTp)(2)Fe-2(CN)(6)Ni[(1,3,2S)-chxn](2)} (2) [chxn = 1,2-diaminocyclohexane; MeTp = methyltris(pyrazolyl)borate), have been synthesized and structurally characterized. Ferroelectric and magnetic measurements reveal that they are rare examples of metal-organic compounds bearing ferroelectricity and intramolecular ferromagnetic interactions.