AbstractPure voltage-controlled magnetism, rather than a spin current or magnetic field, is the goal for next-generation ultralow power consumption spintronic devices. To advance toward this goal, we report a voltage-controlled nonvolatile 90° magnetization rotation and voltage-assisted 180° magnetization reversal in a spin-valve multiferroic heterostructure. Here, a spin valve with a synthetic antiferromagnetic structure was grown on a (110)-cut Pb(Mg1/3Nb2/3)0.7Ti0.3O3 (PMN-PT) substrate, in which only the magnetic moment of the free layer can be manipulated by an electric field (E-field) via the strain-mediated magnetoelectric coupling effect. As a result of selecting a specified PMN-PT substrate with defect dipoles, nonvolatile and stable magnetization switching was achieved by using voltage impulses. Accordingly, a giant, reversible and nonvolatile magnetoresistance modulation was achieved without the assistance of a magnetic field. In addition, by adopting a small voltage impulse, the critical magnetic field required for complete 180° magnetization reversal of the free layer can be tremendously reduced. A magnetoresistance ratio as large as that obtained by a magnetic field or spin current under normal conditions is achieved. These results indicate that E-field-assisted energy-efficient in-plane magnetization switching is a feasible strategy. This work is significant to the development of ultralow-power magnetoresistive memory and spintronic devices.