Reduction of CP*2TaCl2 with sodium amalgam in THF under a nitrogen atmosphere results in the formation of the novel complex (CP*2TaCl)(2)(mu-N-2). This dinuclear complex containing a mu-eta(1):eta(1) dinitrogen bridge has been characterized by NMR and X-ray crystallography. The complex possesses a C-2-symmetric structure with each Ta bound to diastereolopic Cp* rings and chloride in addition to the mu-N-2 bridge. The Ta-N and N-N distances of 1.886(10) and 1.23(1)Angstrom, respectively, suggest modest reduction of the dinitrogen moiety. The two Cp* resonances on each Ta center remain inequivalent in solution, even up to 80 degreesC. Addition of hydrogen results in the formation of two isomers of the dihydride complex CP*2TaH2Cl, Under parahydrogen, polarized resonances are observed for the unsymmetrical isomer with adjacent hydrides as the product of H-2 oxidative addition. The symmetric isomer of CP*2TaH2Cl also forms, most likely by isomerization of the unsymmetrical kinetic isomer. The reactivity of (CP*2TaCl)(2)(mu-N-2) was compared to that of the related monomer, CP*2TaCl(THF). The THF adduct yields the same hydrogen addition products, but the reaction is much more facile than for the nitrogen dimer, indicative of the structural integrity of the mu-N-2 complex.