A tunability-improved magnetoelectric (ME) inductor in the symmetrical composite consisting of spinel Ni–Zn ferrite Ni0.8Zn0.2Fe2O4(NZFO) platelet and piezoelectric ceramics Pb(Zr, Ti)O3 (PZT) slab with Metglas foils laminated was fabricated and systemically characterized. To further improve the tunability in conventional ferrite/PZT inductors, a methodology of Metglas foils laminated with high permeability and magnetostriction was introduced, and thus, significant improvement in inductance tunability was realized. Experimental results show that tunability reaches its maximum in Metglas/ferrite/PZT composite at $L = 2$ and $E = 8$ kV/cm application, exhibiting an enhancement factor of 3.25 times relative to NZFO/PZT/NZFO laminate. Therefore, versatile flexibility on tuning methodology as well as the adjustable range was introduced to provide great potentials for practical applications in compact and power-efficient integrated circuits.