The molybdenum oxo-imido complex, [Mo(O)((NBu)-Bu-t)Cl-2(dme)] (1), was obtained from the reaction between [MoO2-Cl-2(dme)] and [Mo((NBu)-Bu-t)(2)Cl-2(dme)]. Reactions between [Mo(O)(NR)Cl-2(dme)] (where R = Bu-t or 2,6-(Pr2C6H3)-Pr-i) and the disodium Schiff base compounds Na-2(3,5-Bu-t(2))(2)salen, Na-2(3,5-Bu-t(2))(2)salpen, and Na-2(7-Me)(2)salen afforded the first oxo-imido transition metal Schiff base complexes: [Mo(O)((NBu)-Bu-t){(3,5-Bu-t(2))(2)salen}] (2), [Mo(O)((NBu)-Bu-t){(3,5(t)Bu(2))(2)salpen}] (3), and [Mo(O)(N-2,6-(Pr2C6H3)-Pr-i){(7-Me)(2)salen}] (4), respectively. The compounds [Mo((NBu)-Bu-t)(2){(3,5(t)Bu(2))(2)salpen}] (5) from [Mo((NBu)-Bu-t)(2)((NHBu)-Bu-t)(2)] and [Mo(N-2,6-(Pr2C6H3)-Pr-i)(2){(7-Me)(2)salen}] (6) from [Mo(N-2,6-(Pr2C6H3)-Pr-i)(2)((NHBu)-Bu-t)(2)] (7) are also reported. Compounds 1-7 were characterized by NMR, IR, and FAB mass spectroscopy while compounds 3, 4, and 5 were additionally characterized by X-ray crystallography. In conjunction with (BuOOH)-Bu-t as oxidant, compound 3 is a catalyst for the oxidation of benzyl alcohol to benzaldehyde and cis-cyclooctene and 1-octene to the corresponding epoxides.