Single molecule magnets (SMMs) containing dysprosium‐phosphorus bonding are rare due to great challenges in constructing the bonding between hard lanthanide ions and soft phosphorus donors. Here we successfully isolated a novel mononuclear bis‐Cp* dysprosium compound, Cp*2Dy[η‐CH(PPh2)2]·C7H8 (1‐Dy), via the salt metathesis reactions of Cp*2Dy(BPh4) and K[(PPh2)2CH] in THF (Cp* = pentamethylcyclopentadienyl). The magnetic investigations indicate its strong SMM behavior evidenced by the open magnetic hysteresis loops below 6 K and the high effective barrier of 300 cm‐1. This could be ascribed to weak dative DyIII‐P bonds at equatorial sites in such [Cp2DyX]‐type (X = auxiliary donors) complexes.