Addition of 4 equiv of LiN=C(t)u(2) to FeCl2 in Et2O/THF results in the formation of [Li(THF)](2)[Fe(N-C(t)u(2))(4)] (1). Oxidation of 1 with 0.5 equiv of I-2 in Et2O/DME yields [Li(DME)][Fe(N=CSu(2))(4)] (2) in moderate yield. Both 1 and 2 are high spin and exhibit tetrahedral geometries in the solid state. Oxidation of 1 with 1 equiv of I-2 in Et2O yields Fe(N-C(t)u(2))(4) (3) in good yield. Surprisingly, complex 3 exhibits a diamagnetic ground state and a nearly square planar geometry about the Fe center.