The use of the N-heterocyclic carbene (NHC) ligands 1,3-bis(2',6'-diethylphenyl)-4,5-(CH2)(4)-imidazol-2-ylidene (cyIDep), 1,3-bis(2',6'-diethylphenyl)-imidazolin-2-ylidene (sIDep), and its N-mesityl analogue sIMes enables the preparation of the two-coordinate homoleptic iron(I)-NHC complexes [(cyIDep)(2)Fe][BAr4F] (3, Ar-F denoted for 3,5-di(trifluoromethyl)phenyl) and [(sIDep)(2)Fe][BAr4F] (4) and the T-shaped iron(I)-NHC complex [(sIMes)(2)Fe(THF)]-[BPh4] (5, THF = tetrahydrofuran). Complexes 3-5 were prepared via the sequential protocol of control reduction of iron(II) dihalides by KC8 in the presence of the corresponding NHC ligands followed by halide-abstraction with NaBAr4. Spectroscopic characterization, including single-crystal X-ray diffraction studies and Fe-57 Mossbauer spectroscopy, in combination with density functional theory calculations, suggest their high-spin nature. Solution property study (absorption spectroscopy and cyclic voltammetry) indicates that 3 and 5 keep their corresponding two- and three-coordinate nature in THF solution, and 4 might reversibly coordinate a THF molecule to form, presumably, the T-shaped species [(sIDep)(2)Fe(THF)][BAr4F]. The isolation of 3 and 4 demonstrates the accessibility of homoleptic two-coordinate iron(I)-NHC complexes.