Fabrication of metal oxide thin films with thickness control of nanometer precision is an important technology that leads to wide practical applications. The present study demonstrates that a surface sol-gel process, composed of chemisorption of alkoxide, rinsing, hydrolysis, and drying, is a superior technique for the preparation of ultrathin metal oxide films with molecular precision. The simplicity of this process should be a great advantage in commercial production of nanosized oxide films.