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Vanadium oxide (VOx) compounds feature various polymorphs, including V2O5 and VO2, with attractive temperature-tunable optical and electrical properties. However, to achieve the desired material property, high-temperature post-deposition annealing of as-grown VOx films is mostly needed, limiting its use for low-temperature compatible substrates and processes. Herein, we report on the low-temperature hollow-cathode plasma-enhanced atomic layer deposition (ALD) of crystalline vanadium oxide thin films using tetrakis(ethylmethylamido)vanadium and oxygen plasma as a precursor and coreactant, respectively. To extract the impact of the type of plasma source, VOx samples were also synthesized in an inductively coupled plasma-enhanced ALD reactor. Moreover, we have incorporated in situ Ar-plasma and ex situ thermal annealing to investigate the tunability of VOx structural properties. Our findings confirm that both plasma-ALD techniques were able to synthesize as-grown polycrystalline V2O5 films at 150 °C. Postdeposition thermal annealing converted the as-grown V2O5 films into different crystalline VOx states: V2O3, V4O9, and VO2. The last one, VO2 is particularly interesting as a phase-change material, and the metal-insulator transition around 70 °C has been confirmed using temperature-dependent x-ray diffraction and resistivity measurements.