I–II–VI Ternary chalcopyrite semiconductors of Cu 1− x Zn 1− y Se 2− δ (Cu3Zn3Se) were successfully fabricated by the atmospheric pressure metal-organic chemical vapor deposition method for the first time. Four major peaks of (112), (220)/(204), (312)/(116), and (400), accompanied by three minor peaks of (103), (211) and (301) were observable in the X-ray diffraction spectra. In particular, the presence of those latter low-intensity peaks featured the formation of the chalcopyrite type Cu3Zn3Se compound. Typical absorption coefficients of the films produced were found to vary from 2.75 × 10 4 cm − 1 to 5.75 × 10 4 cm − 1 over all visible light range and from the same optical absorption spectra the energy gap of the material was extracted to be about 2.02 eV. Moreover, the photoluminescence measurement conducted at room temperature also exhibited a strong orange-colored emission line at 1.94 eV, which further confirmed that the Cu3Zn3Se ternary compound has been prepared. In addition, the cross-sectional and top-view scanning electron microscopy images characterized the fabricated Cu3Zn3Se compound as a polycrystalline film of thickness about 1–1.3 μm and consisting of 1–2.5 μm sized grains.