A method of producing an Ln1−yMyCuOX single-crystal thin film, wherein Ln is at least one selected from the group consisting of lanthanide elements and yttrium, 0<y<1, and M is at least one selected from the group consisting of Mg, Ca, Sr, Ba and Zn and X is at least one selected from the group consisting of S, Se and Te, said method comprising the steps of:
- growing a base thin film on a single-crystal substrate;
- depositing an amorphous or polycrystalline Ln1−yMyCuOX thin film on said base thin film to form a laminated film;
- enclosing said laminated film in a closed vacuum environment, and
- then annealing said laminated film at a high temperature of 500° C. or more in said vacuum environment.