Atomic-layer chemical-vapor-deposition (AL-CVD) of SiO2 has been achieved by cyclic exposures of CH3OSi(NCO)(3) and H2O2 at room temperature. The deposition rate was saturated at about 2.0 Angstrom/cycle i.e., equal to the ideal quasi-monolayer/cycle. The surface roughness after 100 deposition cycles was found to be less than +/-10 Angstrom by atomic force microscopy (AFM). Film properties were also evaluated by auger electron spectroscopy (AES), X-ray photoemission spectroscopy (XPS), and Fourier transform IR (FT-IR) spectroscopy.