A Fe-parallel to-based metal-organic framework (MOF), {[Fe-2(pbt)(2)(H2O)(2)]center dot 2H(2)O}(n), undergoes an irreversible dehydration, which triggers changes in the catalytic and magnetic properties of the MOF. These property changes are attributed to the high-spin to low-spin transition of 7.1% center Fe-parallel to, which is demonstrated by Fe-57 Mossbauer, X-ray photoelectron spectroscopy, and UV/vis absorption spectra.