Heteroleptic bis(tert-butylimido)bis(N,N′-diisopropylacetamidinato) compounds of molybdenum and tungsten are introduced as precursors for atomic layer deposition of tungsten and molybdenum oxide thin films using ozone as the oxygen source. Both precursors have similar thermal properties but exhibit different growth behaviors. With the molybdenum precursor, high growth rates up to 2 Å/cycle at 300 °C and extremely uniform films are obtained, although the surface reactions are not completely saturative. The corresponding tungsten precursor enables saturative film growth with a lower growth rate of 0.45 Å/cycle at 300 °C. Highly pure films of both metal oxides are deposited, and their phase as well as stoichiometry can be tuned by changing the deposition conditions. The WO_x films crystallize as γ-WO₃ at 300 °C and above, whereas the films deposited at lower temperatures are amorphous. Molybdenum oxide can be deposited as either amorphous (≤250 °C), crystalline suboxide (275 °C), a mixture of suboxide and α-MoO₃ (300 °C), or pure α-MoO₃ (≥325 °C) films. MoO_x films are further characterized by synchrotron photoemission spectroscopy and temperature-dependent resistivity measurements. A suboxide MoO_x film deposited at 275 °C is demonstrated to serve as an efficient hydrogen gas sensor at a low operating temperature of 120 °C.