We comparatively investigate the influence of various high-permeability alloys on the hysteretic and remanent resonant magnetoelectric (ME) response in a composite of magnetostrictive nickel (Ni) and piezoelectric Pb(Zr1−x, Tix)O3 (PZT). In order to implement this comparative research, Co-based amorphous alloy (CoSiB), Fe-based nanocrystalline alloy (FeCuNbSiB) and Fe-based amorphous alloy (FeSiB) are used according to different magnetostriction (λs) and saturation magnetization (μ0Ms) characteristics. The bending and longitudinal resonant ME voltage coefficients (αME,b and αME,l) are observed comparatively for CoSiB/Ni/PZT, FeCuNbSiB/Ni/PZT, and FeSiB/Ni/PZT composites. The experimental data indicate that the FeSiB/Ni/PZT composite has the largest remanent self-biased αME,b and αME,l due to the largest magnetic grading of λs and μ0Ms in the FeSiB/Ni layer. When the number of FeSiB foils is four, the maximum remanent αME,b and αME,l at zero bias magnetic field are 57.8 V/cm·Oe and 107.6 V/cm·Oe, respectively. It is recommended that the high-permeability alloy is supposed to have larger λs and μ0Ms for obtaining a larger remanent self-biased ME responses in ME composite with high-permeability alloy.