Single crystals of the FeII metal‐organic framework (MOF) with 1,3,5‐benzenetricarboxylate (BTC) as a linker were solvothermally obtained under air‐free conditions. X‐ray diffraction analysis of the crystals demonstrated a structure for FeII‐MOF analogous to that of [Cu3(BTC)2] (HKUST‐1). Unlike HKUST‐1, however, the FeII‐MOF did not retain permanent porosity after exchange of guest molecules. The Mössbauer spectrum of the FeII‐MOF was recorded at 80 K in zero field yielding an apparent quadrupole splitting of ΔEQ = 2.43 mm·s–1, and an isomer shift of δ = 1.20 mm·s–1, consistent with high‐spin central iron(II) atoms. Air exposure of the FeII‐MOF was found to result in oxidation of the metal atoms to afford FeIII. These results demonstrate that FeII‐based MOFs can be prepared in similar fashion to the [Cu3(BTC)2], but that they lack permanent porosity when degassed.