Electric-field driven magnetization switching in ${\mathrm{FePt}/\mathrm{BaTiO}}_3$ (001) is demonstrated through first-principles calculations. The magnetic easy axis of the FePt layer undergoes a transition from an in-plane to perpendicular direction upon ferroelectric polarization switching, a process sensitively controlled by epitaxial strain ($\eta$) with a threshold value $\eta \approx 2\%$. In this phenomenon, a large interfacial magnetoelectric coupling (${\alpha }_I=3.6\times {10}^{-10} \mathrm{G}{\mathrm{cm}}^2/\mathrm{V}$) is responsible, stemming from the orbital reconstruction. In particular, the redistribution of Pt-$d$ orbital occupancy alters spin-orbit coupling, thereby tuning the competition between magnetic anisotropy ($K_i$) and magnetoelastic energy ($b_1$). Our work clarifies the fundamental physics of strain-engineered magnetoelectricity and suggests a concrete pathway for designing ultralow-power voltage-controlled magnetic memory.

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• Magnetic anisotropy
• Magnetoelastic effect
• Magnetoelectric effect
• Ab initio calculations