Using dimethylaluminum hydride as the source gas and an ArF laser as the light source, aluminum thin films with low electrical conductivity were deposited via photochemical reactions. To emphasize surface reactions, vapor pressure was kept low with a t pical value of 6.7×10−3 Pa. The laser energy density was typically 23 mJ/cm2 per pulse. The deposition rate of aluminum films became reasonably high above a substrate temperature of 90 °C and increased thereafter with substrate temperature. The electrical resistivity was about four times greater than the bulk aluminum value. A strongly nonlinear dependence of the deposition rates on laser energy density was observed. The incremental change in thickness per pulse increased with the inverse of the pulse repetition rate, which indicated, together with area selectivity, the importance of surface photolysis of absorbed molecules.