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(Zr 1−x , Ti x )O 3 (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 (λ s ) and saturation magnetization (µ 0 M s ) characteristics. The bending and longitudinal resonant ME voltage coefficients (α ME,b and α ME,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 α ME,b and α ME,l due to the largest magnetic grading of λ s and µ 0 M s in the FeSiB/Ni layer. When the number of FeSiB foils is four, the maximum remanent α ME,b and α ME,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 λ s and µ 0 M s for obtaining a larger remanent self-biased ME responses in ME composite with high-permeability alloy.