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ZnO layers were grown on (111) GaAs substrates by laser molecular epitaxy at substrate temperatures between 200 and 550°C. X-ray diffraction analysis revealed that c-axis of ZnO epilayer with a wurtzite structure is perpendicular to the substrate surface. X-ray rocking curves and Raman spectroscopy showed that the crystal quality of ZnO epilayers depends on the substrate temperature during the growth. Strong near-band-edge emission in the UV region without any deep-level emissions was observed from the ZnO epilayers at room temperature. The results indicate that laser molecular beam epitaxy is a promising growth method for obtaining high-quality ZnO layers on (111) GaAs substrates.