Single‐crystalline antiferromagnetic artificially layered [Ni/Mn] films of different thicknesses, covered by ferromagnetic Co layers, are deposited on . Their structural and magnetic properties are characterized by low‐energy electron diffraction (LEED) and magneto‐optical Kerr effect, respectively, and compared with disordered alloy films with the same Ni/Mn ratio and the same film thickness. LEED intensity‐versus‐energy curves show that the perpendicular interatomic lattice distance is decreased in the artificially layered [Ni/Mn] samples in comparison to the disordered alloy films. At the same time, the artificially layered [Ni/Mn] films exhibit higher coercivity and exchange bias of the adjacent Co layer compared to those of . This is discussed as a consequence of the different interatomic lattice distance, presumably caused by an ordered buckling in the artificially layered [Ni/Mn] samples, leading to a stronger interlayer exchange coupling.