Surface morphology of aluminum thin films grown by metallorganic chemical vapor deposition has been improved by growing aluminum/titanium nitride multilayers. When the aluminum films were deposited continuously, the reflectance vs. deposition thickness curves showed a maximum reflectance at the completion of coalescence of islands, and then showed a gradual decay with increasing aluminum thickness because of nonuniform grain growth. By inserting 1 nm titanium nitride layer grown by atomic layer deposition on aluminum layer at the maximum reflectance, the reflectance was recovered again to the peak reflectance like a sinusoid waveform. Therefore, without considerable loss of electrical conductivity surface smoothness of aluminum films has been able to be achieved by repeating the aluminum/titanium nitride multilayer depositions.