The 1,2-diaza-4-phospholide (dp⁻) dipotassium ate complexes of chromium(II) {[(η¹-N-3,5-tBu₂dp)₄Cr][(η⁵-(N,N,C,C,P))₂-K(η¹-O-THF)₂]₂} (5) and {[(η¹-N-3,5-Ph₂dp)₄Cr][(η⁵-(N,N,C,C,P))₂-K(η¹-O-THF)₂]₂}_∞ (6) were synthesized and characterized by X-ray single crystal structure analysis. Complex 5 with a near-square planar geometry at the chromium(II) ion was unambiguously characterized by the high field electron paramagnetic resonance (HF-EPR) technique and magnetic measurements, revealing that it is a field-induced single-molecule magnet (SMM).