Magnetoelectric coupling capable of electrically switching magnetic anisotropy is essential for the development of next-generation magnetic memory and spintronic devices. However, achieving strong magnetoelectric coupling in multiferroic heterostructures is often hindered by the weak and unstable ferroelectricity of conventional ferroelectrics at the ultrathin limit. Here, we propose a strategy based on bilayer aluminum nitride (AlN), a sliding ferroelectric in which opposite out-of-plane polarization states are realized in the AB- and AC-stacked configurations and can be reversibly switched via interlayer sliding, thereby overcoming the scaling limitations of conventional ferroelectrics. Moreover, we combine bilayer AlN with the ferromagnetic monolayer 1T-${\mathrm{MnS}}_2$ to construct an ${\mathrm{MnS}}_2$/bi-AlN multiferroic heterostructure. We find that polarization switching in bilayer AlN strongly modifies the magnetic anisotropy energy (MAE) of the ${\mathrm{MnS}}_2$ layer, where the reversal of AlN sliding ferroelectricity leads to a switching of the magnetic easy axis, while the MAE changes by more than 700%. Furthermore, orbital-projected analysis reveals that this strong magnetoelectric coupling originates from polarization-driven interfacial charge transfer, which modifies orbital hybridization and the crystal field environment at the magnetic ion sites. These results demonstrate that sliding-ferroelectric-based heterostructures provide an effective route toward strong magnetoelectric coupling and electrically switchable magnetic anisotropy, offering opportunities for low-power two-dimensional spintronic devices.

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• Magnetic anisotropy
• Magnetoelectric effect
• Sliding ferroelectricity
• Heterostructures
• Multiferroics
• First-principles calculations