The unconventional π magnetism emerging at the edges of zigzag graphene nanoribbons (ZGNRs) has attracted considerable interest in carbon-based spintronics, motivating extensive efforts to understand and manipulate their spin distributions. Inspired by the recent discovery of electrically switchable ferroelectricity via interlayer sliding in multilayer graphene with more than three layers [L. Yang et al., Phys. Rev. Lett. 131, 096801 (2023)], we propose a nonvolatile and electrically switchable approach to modulate the magnetic properties of the ZGNR through heterostructure engineering with multilayer graphene. Using first-principles calculations, we demonstrate that when the ZGNR is positioned as either a surface layer or an internal layer in ABA stacking with adjacent layers, the stacking-induced charge redistribution creates a sublattice imbalance, leading to spin splitting. Furthermore, this spin splitting can be effectively modulated by polarization reversal through interlayer sliding. Specifically, in-plane polarization reversal is predicted to switch the spin splitting direction, while out of plane polarization reversal may either alter the presence of spin splitting or reverse its direction, depending on the stacking configuration. Our work provides a strategy for ferroelectric control of spin splitting in the ZGNR, demonstrating its potential as a key platform for nanoscale spintronic devices.

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• Ferroelectricity
• Magnetoelectric effect
• 2-dimensional systems
• Elemental materials
• First-principles calculations