The synthesis, characterization, and thermogravimetric analysis of tris(N,N′-di-isopropylacetamidinate)molybdenum(III), Mo(iPr-AMD)₃, are reported. Mo(iPr-AMD)₃ is a rare example of a homoleptic mononuclear complex of molybdenum(III) and fills a longstanding gap in the literature of transition metal(III) trisamidinate complexes. Thermogravimetric analysis (TGA) reveals excellent volatilization at elevated temperatures, pointing to potential applications as a vapor phase precursor for higher temperature atomic layer deposition (ALD), or chemical vapor deposition (CVD) growth of Mo-based materials. The measured TGA temperature window was 200–314 °C for samples in the 3–20 mg range. To validate the utility of Mo(iPr-AMD)₃, we demonstrate aerosol-assisted CVD growth of MoO₃ from benzonitrile solutions of Mo(iPr-AMD)₃ at 500 °C using compressed air as the carrier gas. The resulting films are characterized by X-ray photoelectron spectroscopy, X-ray diffraction, and Raman spectroscopy. We further demonstrate the potential for ALD growth at 200 °C with a Mo(iPr-AMD)₃/Ar purge/300 W O₂ plasma/Ar purge sequence, yielding ultrathin films which retain a nitride/oxynitride component. Our results highlight the broad scope utility and potential of Mo(iPr-AMD)₃ as a stable, high-temperature precursor for both CVD and ALD processes.