The reaction of 2-pyridiyldiphenylphosphine (2) with tetrachloromethane and subsequent dehalogenation of the intermediate chloro phosphonium salt [(CDPPy2)Cl]Cl (3) with tris(1-pyrrolidyl)phosphine results in the formation of a new type of carbodiphosphorane N,C,N pincer ligand, sym-bis(2-pyridyl)tetraphenylcarbodiphosphorane, CDPPy2 (1). It crystallizes in a triclinic crystal system with a crystallographic point group of P1. This neutral double-ylidic N,C,N ligand is capable of stabilizing a wide range of metal coordination polyhedra, varying from square planar [(CDPPy2)PdCl]Cl (4), octahedral mer-[(CDPPy2)TiCl3] (5) and fac-[(CDPPy2)Cr(CO)3] (6) to trigonal-bipyramidal [(CDPPy2)MnCl2] (9) and [(CDPPy2)CoCl2] (10) complexes. Unprecedented dinuclear complexes are formed with molybdenum and nickel carbonyls. 1 reacts with [Mo(CO)3(NCMe)3] to form the symmetric κ3-N,C,N-[(CDPPy2)Mo(CO)3(μ-CO)Mo(CO)3] (7) with one bridging carbonyl next to a bridging central carbon atom with its two lone pairs. In contrast,...