Artificially layered materials of alternating 2–3 nm thick copper and nickel layers have been produced by electrodeposition on oriented single‐crystal copper substrates. X‐ray diffraction examination of thin layers chemically removed from the substrate showed that a coherent, relatively homogeneous coating, with a strong epitaxial relationship, had been produced. In particular, artificially layered Cu‐Ni alloys displaying a textured [110] orientation were obtained by electrodeposition. Noncoherent nucleation leads to the presence of various amounts of randomly oriented alloy grains on all substrates but, in particular, for the [100] orientation.