Epitaxial layers of Cd1−xZnxTe (0.04≤x≤0.62) have been grown on (100) and (111) silicon substrates by a low‐pressure chemical vapor deposition (LPCVD) process. Elemental metals were used as sources of cadmium and zinc and dimethyltelluride was used as a source of tellurium. The characterization of layers by x‐ray diffraction, scanning electron microscope, and scanning electron microscope x‐ray dispersive analysis shows that hot wall LPCVD is a viable technique to grow large‐area epitaxial layers of CdZnTe on different substrates.