AbstractVoltage-induced switching of magnetization, as opposed to current-driven spin transfer torque switching, can lead to a new paradigm enabling ultralow-power and high density instant-on nonvolatile magnetoelectric random access memory (MeRAM). To date, however, a major bottleneck in optimizing the performance of MeRAM devices is the low voltage-controlled magnetic anisotropy (VCMA) efficiency (change of interfacial magnetic anisotropy energy per unit electric field) leading in turn to high switching energy and write voltage. In this work, employing ab initio electronic structure calculations, we show that epitaxial strain, which is ubiquitous in MeRAM heterostructures, gives rise to a rich variety of VCMA behavior with giant VCMA coefficient (~1800 fJ V⁻¹m⁻¹) in Au/FeCo/MgO junction. The heterostructure also exhibits a strain-induced spin-reorientation induced by a nonlinear magnetoelastic coupling. The results demonstrate that the VCMA behavior is universal and robust in magnetic junctions with heavy metal caps across the 5d transition metals and that an electric-field-driven magnetic switching at low voltage is achievable by design. These findings open interesting prospects for exploiting strain engineering to harvest higher efficiency VCMA for the next generation MeRAM devices.