Ferrovalleytricity switching is the most crucial operation in valleytronics. In current valleytronic research, it is predominately realized by magnetic field, which is not favored in terms of efficiency. Here, we propose a mechanism that allows ferrovalleytricity switching fully controlled by voltage pulses. The physics correlates to the peculiar magnetoelectric coupling in multiferroic heterobilayers, where the reversal of ferroelectric polarization reverses interlayer magnetic ground order. We show that such coupling can enable the reversal of spin orientation and consequently the ferrovalleytronic polarization of carriers through purely electric means, thereby achieving electrically switchable ferrovalleytricity. Using first-principles calculations, we further validate this mechanism in the multiferroic heterobilayer ${\mathrm{CuCrP}}_2{\mathrm{S}}_6/{\mathrm{CrBr}}_3$. The significant disparity in magnetic anisotropy of two constitute layers is identified to play a vital role in realizing the mechanism. Our findings establish a promising route toward the electric field control of ferrovalleytricity.

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• First-principles calculations
• Magnetoelectric effect
• Spintronics
• Valley degrees of freedom
• Bilayer films
• Ferroelectrics
• Multiferroics
• Density functional calculations