Zinc acetate-polyethylene (ZnAc2-PE) composite coatings having controllably optical properties were synthesized in vacuum by electron beam dispersion (EBD) method with pulse laser assistant (PLA), using the mixture of ZnAc2 and PE as target materials. The composition, structure, morphology, optical and photoluminescence properties of the coatings were examined with respect to the laser assistant and post-annealing temperature (100-200 A degrees C). The annealed coatings at 200 A degrees C possessed a dominant wurtzite structure of ZnO. The ZnAc2-PE coatings exhibited elongated agglomerates (nanorods-like) of the length 120 nm, which was largely different from the spherical particles in single ZnAc2 or PE coatings. Studies by infrared spectroscopy and X-ray photoelectron spectroscopy revealed that PLA and PE influence the molecular structure and bond compositions of ZnAc2 coatings due to the change of active gas phase from the decomposition of target components during EBD. UV-Vis spectra showed that the annealed ZnAc2-PE coating with high transparent exhibits a characteristic absorption of ZnO at 361 nm and has a blueshift of the band gap up to 0.23 eV compared to ZnAc2 coatings. This resulted from the passivation effect of PE on the oxidation and decomposition of coatings during annealing. The annealed ZnAc2-PE coating with PLA exhibited a strong UV emission and a weak defect-related blue-luminescence emission. The present synthesis method of the inorganic-organic coatings may be envisioned to provide a promising way for fabricating high-performance UV detectors and optoelectronic devices.