We describe pyrolytic laser assisted chemical vapor deposition of Al from dimethylethylamine‐alane with 514‐nm radiation from an Ar ion laser. High purity Al lines with resistivity close to bulk Al are reported for a range of operating conditions. The relationship between operating parameters and materials properties of the deposited lines is delineated. Results from deposition on different substrates, Pt, Au, W, and Si, provide insight into thermal and nucleation effects in the laser writing process. Based on the observed nucleation behavior, we demonstrate a two‐step fast writing process involving fast laser nucleation of lines, followed by selective chemical vapor deposition of Al on the nucleated pattern.