Controlling unconventional magnetism of graphene, particularly antiferromagnets with ferromagnet-like properties, is crucial for advancing spintronics based on graphene. Here, through first-principles calculations and experimental measurement, we propose sliding ferroelectricity and magnetoelectric coupling in specifically stacked van der Waals heterostructures composed of zigzag graphene nanoribbons (ZGNRs) encapsulated between hexagonal boron nitride (h-BN) layers. The designed h-BN/ZGNR/h-BN heterostructure exhibits spontaneous out-of-plane polarization due to stacking-induced inversion symmetry breaking, enabling bistable polarization states reversible via interlayer sliding with an ultralow energy barrier. Crucially, this polarization lifts degeneracy between the antiferromagnetically coupled edge states of ZGNRs, inducing pronounced spin splitting in the electronic band structure. The resulting spin-polarized conductivity is electrically tunable through sliding-mediated polarization switching. This work establishes a new multiferroic platform based on graphene nanoribbon.

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• Edge states
• Ferroelectricity
• First-principles calculations
• Magnetoelectric effect
• Spintronics
• Graphene
• Nanoribbon