ZnO thin films were deposited on Si(100) substrates at low temperatures (44℃~210℃) by atomic layer deposition using DEZn (diethyl zinc) and water as precursors. The film thickness was measured by ellipsometry calibrated with cross-sectional TEM. The phase formation, microstructure evolution, UV-absorbance, and chemical composition changes were examined by XRD, SEM, AFM, TEM, UV-VIS-NIR, and AES, respectively. A uniform amorphous ZnO layer was formed even at 44℃ while stable crystallized ZnO films were deposited above 90℃. All the samples showed uniform surface roughness below 3 nm. Fully crystallized ZnO layers with a band-gap of 3.37 eV without carbon impurities can be formed at substrate temperatures of less than 90℃.