Addition of an equal molar quantity of R(-) (R = Me, SiMe(3)) to complex (Nacnac)Ti=NAr(OTf) (Nacnac(-) = [ArNC(tBu)](2)CH, Ar = 2,6-iPr(2)C(6)H(3)) forms the imido alkyl (Nacnac) Ti=NAr(R), which can be readily protonated to afford [(Nacnac)Ti=NAr(L)](+) (L = THF, Et(2)O, eta(1)-C(6)H(5)NMe(2)), or treated with B(C(6)F(5))(3) to afford the zwitterion (Nacnac) Ti=NAr(mu-CH(3))B(C(6)F(5))(3).