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In the complex cation of the title compound, [Fe(C27H41N10O3)](PF6)2, the tripodal tris{4-[1-(2-methoxyethyl)imidazol-2-yl]-3-azabut-3-enyl}amine ligand is coordinated to an FeII ion through the nitrogen atoms of three imidazole and three imino groups. The Fe atom exhibits a distorted octahedral geometry. In the crystal, l and d antipodes are arranged in layers in the bc plane. Weak C...F and C—H...F/O contacts exist between the ligands of the complex cation and the PF6− anions, generating a three-dimensional network. At 120 K, the FeII ion is in a low-spin state, with an average Fe—N bond distance of 1.970 (2) Å. On heating, the FeII ion converts to the high-spin state, as demonstrated by magnetic susceptibility measurements.