The laser‐induced deposition of high‐purity aluminum metal has been achieved by pyrolytic decomposition of trimethylamine aluminum hydride. The chemical structure of the precursor affords a high ambient vapor pressure which results in rapid rates of aluminum film formation. In addition, the precursor is nonpyrophoric, in contrast to other trialkylaluminum precursors. These combined chemical and physical properties make trimethylamine aluminum hydride an ideal precursor for laser‐induced chemical vapor deposition of aluminun films.