We report on a two‐step process for the patterning and growth of aluminum films from the metallorganic source gas dimethylaluminum hydride (DMAlH). In particular, ultraviolet light from a cw or pulsed laser source is used to generate a seed layer for selective chemical vapor deposition of aluminum conductors. The dependence of growth selectivity on the temperature and substrate material, the influence of the seed‐layer thickness on film growth, and the process parameters such as temperature and pressure, that yield high purity aluminum, are presented. This technique has been applied to two applications with different materials requirements: final metallization of a complementary metal–oxide‐semiconductor gate array in silicon, and electrode formation for GaAs/AlGaAs integrated optical modulators.