Achieving precise and nonvolatile electrical control of spin represents a fundamental yet long-standing challenge in spintronics. In this work, we demonstrate that bilayer altermagnets with sliding ferroelectricity give rise to a distinct form of sliding multiferroicity, thereby establishing a pathway for precise and nonvolatile electrical spin manipulation. Through a combination of symmetry analysis and first-principles calculations, we identify bilayer Ca(CoN)${}_2$ as a representative system, in which sliding between layers reconstructs the stacking order and switches the spontaneous polarization with an ultralow energy barrier. Unlike conventional gate-controlled schemes, the spin-layer coupling in this sliding multiferroic arises intrinsically from the spontaneous electrical and layer polarizations, eliminating the need for a sustained gate field to maintain the spin state. The two distinct multiferroic phases further exhibit a fully switchable anomalous Hall effect and a pronounced magneto-optical response, providing potential experimental signatures. These findings highlight the promise of leveraging sliding-mediated coupling between unconventional magnetism and stacking order to realize electrically programmable two-dimensional multiferroics.

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• Spintronics
• Valleytronics
• Altermagnets
• Magnetic systems
• Multiferroics
• First-principles calculations