Al2O3 layers with thicknesses in the 25–120 nm range were deposited by plasma enhanced atomic layer deposition at 70 °C. Trimethylaluminum was used as organometallic precursor, O2 and H2O as oxidant agents and Ar as a purge gas. The deposition cycle consisted of 50 ms TMA pulse/10 s purge time/6 s of plasma oxidation at 200 W/10 s purge time. The optical constants and thicknesses of the grown layers were determined by spectroscopic ellipsometry, while the roughness was measured by atomic force microscopy, giving RMS values in the 0.29–0.32 nm range for films deposited under different conditions and having different thicknesses. High transmittance, ~90%, was measured by UV–Vis spectroscopy. X-ray photoelectron spectroscopy revealed that, with both types of oxidants, the obtained films are close to stoichiometric composition and, with high purity, no carbon was detected. Electrical characterization showed good insulating properties of both types of films, though the H2O oxidant leads to better I-V characteristics.