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Zn1−xCdxO films are grown on c-sapphire substrates by laser molecular beam epitaxy (LMBE) at different temperatures. Their crystallographic structures, compositions, surface electronic structures are investigated. The a-axis lattice constant of Zn0.95Cd0.05O is 3.20 Å. Moreover, the epitaxial relationship shows a 30°-in-plane rotation of the film with respect to the c-sapphire substrate. When the substrate temperatures arrives at 500°C, the in situ reflection high-energy electron diffraction (RHEED) pattern of ZnCdO film shows sharp streaky pattern. The maximum Cd content of ZnCdO film grown at low substrate temperatures increases up to about 29.6 at.%, which is close to that of the ceramic target. In situ ultraviolet photoelectron spectroscopy (UPS) measurements demonstrate that ZnCdO film exhibits intense peaks at 4.7 eV and 10.7 eV below the Fermi level, which are assigned to the O 2p and Zn 3p states. Energetic distance between Zn 3d and Cd 4d is 0.60 eV. Above 470 nm, the thin film shows excellent optical transmission. [ABSTRACT FROM AUTHOR]