The bis(imido) complex MoCl2(Nmes)(2)(dme) (1) (mes = 2,4,6-trimethylphenyl, dme = 1,2-dimethoxyethane) has been used as the starting material for the preparation of the compounds (L-OEt)Mo(Nmes)(2)Cl (2) (L-OEt = (eta-C5H5)Co{P(O)(OEt)(2)}(3)) and Mo(Nmes)(2)(acac)(2) (5), as well as for the synthesis of the mixed oxo-imido MoCl2(Nmes)(O)(dme) (6), the latter reaction involving conproportionation of 1 and MoCl2(O)(2)(dme). Similarly, the paramagnetic mono(imido) species Mo(Nmes)Cl-3(dme) (11) can also be obtained from 1 by interaction with MoCl4(THF)(2) (THF = tetrahydrofuran) in refluxing dme. Compounds 6 and 11 are suitable sources for the synthesis of other diamagnetic mixed oxo-imido and paramagnetic mono(imido) compounds, respectively. Three of the newly synthesized complexes, namely, (L-OEt)Mo(Nmes)(2)Cl (2), (L-OEt)Mo(Nmes)Cl-2 (12), and MoCl3(Nmes)(depe) (14) (depe = Et2PCH2CH2PEt2) have been characterized by X-ray crystallography.