Bis(tert-butylimido)-bis(diethylamido)molybdenum [(, possible precursors for atomic layer deposition (ALD) of molybdenum nitride, are synthesized and characterized. Calorimetric studies are carried out to examine the thermal stability of the new precursor candidates. For the diethylamido complex, sufficient thermal stability is found, ALD tests are performed, and satisfactory parameters for controlled growth are identified. Films grown from bis(tert-butylimido)-bis(diethylamido)molybdenum and ammonia are amorphous, smooth, and conformal. The di-isopropylamido complex shows thermal instability and a very low synthetic yield, hence it is not tested in ALD. Possible decomposition reactions of the precursors are studied by density functional theory (DFT) calculations. The computational results support the low thermal stability of di-isopropylamido complex found through calorimetric studies.