Tailoring the spin orientation at the atomic scale has been a key task in spintronics technology. While controlling the out-of-plane to in-plane spin orientation has been achieved by a precise control of the perpendicular magnetic anisotropy at atomic layer thickness level, a design and control of the in-plane magnetic anisotropy has not yet been well developed. On well aligned atomic steps of a 6° vicinal Cu(001) surface with steps parallel to the [110] axis, we grow Py/Ni overlayer films epitaxially to permit a systematic exploration of the step-induced in-plane magnetic anisotropy as a function of both the Py and the Ni film thicknesses. We found that the atomic steps from the vicinal Cu(001) induce an in-plane uniaxial magnetic anisotropy that favors both Py and Ni magnetizations perpendicular to the steps, opposite to the behavior of Co on vicinal Cu(001). In addition, thickness-dependent study shows that the Ni films exhibit different magnetic anisotropy below and above ~6 ML Ni thickness.