In this work, a series of specimens was prepared by the casting method. Sharp cube-textured substrates were processed by heavy cold rolling and recrystallization annealing (i.e., the rolling-assisted biaxially textured substrates (RABiTS) method). Both the rolling and the recrystallization texture in the alloy tapes were investigated by X-ray diffraction and electron back-scatter diffraction, respectively. The results showed that a strong copper-type deformation texture was obtained in the heavy cold-rolled substrate. In addition, the recrystallization annealing process was found to be very important for the texture transition in the Cu–Ni alloy substrates. The cube texture content in the Cu60Ni40 alloy substrates reached 99.7% (≤10°) after optimization of the cold-rolling procedure and the recrystallizing heat-treatment process, whereas the content of low-angle grain boundaries (from 2° to 10° misorientation) in the substrate reached 95.1%.