Treatment of (TTP)Ti(η2-RC⋮CR) (R = Et or Ph) with PhNNPh results in formation of the azobenzene adduct (TTP)Ti(η2-PhNNPh) (1) in good isolated yield. Complex 1 reacts with (TTP)Ti(η2-RC⋮CR) at elevated temperatures to cleanly afford 2 equiv of the phenylimido compound, (TTP)TiNPh (2). The azobenzene complex, 1, is also formed in low yields by the reaction of the (TTP)TiNPh (2) with excess 1,2-diphenylhydrazine. The electrochemistry of the azobenzene adduct (1) and the phenylimido complex (2) is investigated by cyclic voltammetry experiments.