The stable diphosphatetrahedrane, (tBuCP)(2), was isolated only recently, and its coordination chemistry has been little explored so far. Herein we report the synthesis of [Ni{eta(2)-(tBuCP)(2)}(3)] (1) by CO substitution of Ni(CO)(4) with (tBuCP)(2). Single-crystal X-ray diffraction studies revealed that 1 features three intact diphosphatetrahedrane molecules coordinated via their P-P bonds to a single nickel(0) atom. Multinuclear NMR studies suggest that the structure of 1 is retained in solution. The bonding situation is analysed using quantum chemical methods. The coordination behavior of (tBuCP)(2) is compared to the isoelectronic P-4 molecule, which scarcely forms complexes of intact P-4 tetrahedra.