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The reaction of LiP(H)B(N i Pr 2 )[N(SiMe 3 ) 2 ].DME with Cp 2 ZrCl 2 in a 2:1 ratio yields the metallodiphosphane Cp 2 Zr{P(H)B(N i Pr 2 )[N(SiMe 3 ) 2 ]} 2 (3a). Combination of 3a with Mo(CO) 4 (norbornadiene) provides the adduct Cp 2 Zr{P(H)B(N i Pr 2 )[N(SiMe 3 ) 2 ]} 2 .Mo(CO) 4 (4a) in which the metallo-diphosphane 3a acts as a chelating ligand. The compounds have been characterized by spectroscopic methods and the molecular structures of 3a and 4a have been determined by single-crystal X-ray diffraction methods. The chemical and structural features are compared and contrasted with related metallo-diphosphanes that contain organic substituents on the diphosphane P atoms.