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Epitaxial growth of cadmium sulfide on indium phosphide monocrystals has been achieved by using chemical deposition from cadmium ammonia‐thiourea aqueous solutions. The epitaxial growth takes place on InP (1¯1¯1¯) substrates with the c axis of hexagonal CdS perpendicular to the surface. The epitaxy relations are determined by means of electron diffraction techniques. The deposition conditions appear to be flexible with reaction temperatures ranging from 60 to 90 °C, and growth rates about 0.1–0.5 μm h-1.