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Single‐crystal layers of ZnS have been grown on GaP substrates in a hydrogen transport system. In order to clarify the doping effects of In on the growth behavior, some In‐doping experiments with various doping processes are performed. The reversal in the orientation dependence of the growth rate and the improvement of the crystallinity of the epitaxial layers are caused by the existence of In atoms and/or In compounds at the growing surface of ZnS. The In atoms and/or In compounds which exist at the interface between the GaP substrate and ZnS epitaxial layer are shown to have no significant effect on the growth behavior.