The complex [Fe{HC(3-Mepz)(2)(5-Mepz)}(2)](BF4)(2) (pz = pyrazolyl ring) has been prepared by the reaction of HC(3-Mepz)(2)(5-Mepz) with Fe(BF4)(2)center dot 6H(2)O. The solid state structures obtained at 294 and 150 K show a distorted iron(II) octahedral N-6 coordination environment with the largest deviations arising from the restrictions imposed by the chelate rings. At 294 K the complex is predominately high-spin with Fe-N bond distances averaging 2.14 angstrom, distances that are somewhat shorter than expected fora purely high-spin iron(II) complex because of the presence of an admixture of about 80% high-spin and 20% low-spin iron(II). At 294 K the twisting of the pyrazolyl rings from the ideal C-3v symmetry averages only 2.2 degrees, a much smaller twist than has been observed previously in similar complexes. At 150 K the Fe-N bond distances average 1.99 angstrom, indicative of an almost fully low-spin iron(II) complex; the twist angle is only 1.3 degrees, as expected fora complex with these Fe-N bond distances. The magnetic properties show that the complex undergoes a gradual change from low-spin iron(II) below 85 K to high-spin iron(II) at 400 K. The 4.2 to 60 K Mossbauer spectra correspond to a fully low-spin iron(II) complex but, upon further warming above 85 K, the iron(II) begins to undergo spin-state relaxation between the low- and high-spin forms on the Mossbauer time scale. At 155 and 315 K the complex exhibits spin-state relaxation rates of 0.36 and 7.38 MHz, respectively, and an Arrhenius plot of the logarithm of the relaxation rate yields an activation energy of 670 +/- 40 cm(-1) for the spin-state relaxation.