We propose an asymmetric bilayer structure in which the magnetic remanence (MR) is controlled by the in-plane strain of the top NiFe2O4 (NFO) layer epitaxially constrained by the bottom Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) substrate. In this asymmetric structure, an electric-field-induced giant piezoelectric strain from the bottom PMN-PT layer is effectively transferred to the top NFO layer. We have shown that the room-temperature magnetic remanence (MR) of the 100-nm-thick NFO layer is enhanced by 46% when an electric-field-induced in-plane compressive strain is about −0.1%. Synchrotron x-ray absorption near edge structure study supports a scenario of the cation-charge redistribution between Ni2+ and Fe3+ ions under the condition of an electric-field-induced in-plane compressive strain.