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II‐VI compound semiconductors, ZnS, ZnSe, CdS, CdSe, and CdTe, were grown epitaxially on (111) and (100) InP and GaAs substrates by excimer laser ablation. All of these films have good crystalline quality (fully in‐plane aligned) and mirror‐like surface morphology. It was found that, on (111)‐oriented substrates, CdS and CdSe films were in the hexagonal phase with the c axis perpendicular to the surface, while ZnS and ZnSe films were in the cubic phase. The films grown on (100)‐oriented substrates were all cubic. These high quality films should be useful in optoelectronics applications. © 1994 American Institute of Physics.