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Single α-phase (AlxGa1−x)2O3 thin films are grown on m-plane sapphire (α-Al2O3) substrates via metalorganic chemical vapor deposition. By systematically tuning the growth parameters including the precursor molar flow rates, chamber pressure, and growth temperature, the epitaxial growth of high-quality phase pure α-(AlxGa1−x)2O3 films (0 ≤ x ≤ 1) is demonstrated with smooth surface morphologies and alloy homogeneities by comprehensive material characterization. The asymmetrical reciprocal space mapping reveals fully relaxed films for α-(AlxGa1−x)2O3 films with x ≤ 0.5. The coherent growth of α-(AlxGa1−x)2O3/α-Al2O3 superlattice structures is demonstrated with abrupt interfaces and uniform Al distribution for higher Al compositions at x = 0.78 in the α-(AlxGa1−x)2O3 layer. The influence of growth parameters, such as growth temperature and chamber pressure, on the phase stabilization and Al incorporation in the α-(AlxGa1−x)2O3 films is investigated. While lower growth temperatures facilitate the phase stabilization of α-Ga2O3 thin films, lower chamber pressure leads to higher Al incorporation in α-(AlxGa1−x)2O3 films. High resolution x-ray photoelectron spectroscopy was utilized for determining the Al compositions and bandgaps of α-(AlxGa1−x)2O3. Furthermore, the evolution of the valance and conduction band offsets at α-Al2O3/α-(AlxGa1−x)2O3 heterojunctions is evaluated with the variation of Al compositions, which reveals the formation of type-I (straddling) band alignment between α-Al2O3 and α-(AlxGa1−x)2O3. [ABSTRACT FROM AUTHOR]