The tungsten nitrido species, [W(mu-N)(CH(2-)t-Bu)(OAr)(2)](2) (Ar = 2,6-diisopropylphenyl), has been prepared in a reaction between the alkylidyne species, W(C-t-Bu)(CH2-t-Bu)(OAr)(2), and organonitriles. The dimeric nature of the nitride was established in the solid state through an X-ray study and in solution through a combination of N-15 NMR spectroscopy and vibrational spectroscopy. Reaction of the nitride with trimethylsilyl trifluoromethanesulfonate afforded the monomeric trimethylsilyl imido species, W(NSiMe3)(CH2-t-Bu)(OAr)(2)(OSO2CF3), which was also characterized crystallographically. The W2N2 core can be reduced by one electron electrochemically or in bulk with metallocenes to afford the radical anion, {n-Bu4N}{W(mu-N)(CH2-t-Bu)(OAr)(2)](2)}. Density functional theory calculations suggest that the lowest-energy allowable transition in [W(mu-N)(CH2-t-Bu)(OAr)(2)](2) is from a highest occupied molecular orbital consisting largely of ligand-based lone pairs into what is largely a metal-based lowest unoccupied molecular orbital.