Abstract: A chalcopyrite compound, for instance, CuInS.sub.2 or CuInSe.sub.2, is prepared by subjecting a thin film containing copper metal, indium metal, and an indium compound or a compound which contains both indium and copper, selected from the group consisting of oxides, sulfides and selenides, with heat under a reducing atmosphere containing at least one of the Group VIb element or under an atmosphere containing a reducing compound of at least one of the Group VIb element, thereby converting said thin film into a chalcopyrite compound.