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A vertically aligned ZnO/ZnS core/shell nanowire array with type II band alignment was directly synthesized on an indium-tin-oxide glass substrate and the photovoltaic effect of the nanowire array was investigated. The epitaxial relationship, wurtzite (0001) matching zinc-blende (111), was observed in the ZnO/ZnS nano-heterostructure. ZnS coating is found to quench the photoluminescence of ZnO nanowires but enhance the photocurrent with faster response in the photovoltaic device, indicating improvement in charge separation and collection in the type II core/shell nanowire.