The title compound was prepared through a three-step procedure starting with the hydride complex [Mo2Cp2(µ-H)(µ-PtBu2)(CO)4], which was first dehydrogenated through reaction with HBF4·OEt2 to give the unsaturated complex [Mo2Cp2(µ-PtBu2)(CO)4](BF4) (Mo=Mo), which displays a transoid structure according to experimental (Mo-Mo = 2.8283(7) Å) and Density Functional Theory studies. The latter was then reacted with NO to give the dinitrosyl derivative [Mo2Cp2(µ-PtBu2)(CO)2(NO)2](BF4), which in turn was further decarbonylated and nitrosylated upon reaction with [N(PPh3)2]NO2 to give the title nitrosyl-bridged complex (Mo-Mo = 2.905(1) Å). This complex displayed a structure comparable to that of its PCy2-bridged analogue, with similar pyramidalization of the bridging nitrosyl, but a more pronounced folding of the central MoPMoN skeleton and bending of terminal nitrosyls. It also displayed a similar NO bond activation chemistry, as shown by its reactions with HBF4·OEt2 to give the nitroxyl-bridged complex [Mo2Cp2(µ-PtBu2)(µ-k1:η2-HNO)(NO)2](BF4) (HNO = 1.330(8) Å), with P(OEt)3 to give the phosphoraniminate-bridged complex [Mo2Cp2(µ-PtBu2){µ-NP(OEt)3}(NO)2], and with Na(Hg) to give the amide-bridged derivative [Mo2Cp2(µ-PtBu2)(µ-NH2)(NO)2]. Under a nitrogen atmosphere, however, the latter reaction also gave a minor side product identified as the dinitrogen-bridged derivative [Mo4Cp4(µ-PtBu2)2(µ4-N2)(NO)4]. This tetranuclear complex displays a dinitrogen molecule bridging four metal atoms in the novel µ4-k1:k1:k1:k1 coordination mode, with strong metal-nitrogen interactions taking the N2 ligand to the diazendiide (N22-) limit (NN = 1.241(3) Å).