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A new type of graphoepitaxial growth of zinc sulfide (ZnS) crystalline thin films has been investigated. The substrate is polyimide coated with various thin films. It has an inverted pyramidal replica pattern taken from textured (100) single‐crystalline silicon. Crystallinity and growth orientation of films were examined by scanning electron microscopy and x‐ray pole figures. It has been confirmed that the crystal was grown from the bottom of the inverted pyramids. The results show that the graphoepitaxial effects are strongly sensitive to the ability of the semiconductor to wet the substrate coating materials at the nucleation temperature. The controllability of the crystallographic orientation normal to the substrate by the synthetic pattern is more than 85% in the present technology status.