We present a strategy for realizing the nonvolatile electrical control of noncollinear magnetism based on first-principles calculations. We confirm that the VAl2S4 monolayer, a rare two-dimensional type-II multiferroic material, shows an in-plane noncollinear 120°-ordered antiferromagnetic ground state and spin spiral order induced out-of-plane ferroelectricity. In VAl2S4 bilayers, we clarify the spin spiral chirality–sliding ferroelectricity locking effect, which enables flexible electrical switching of noncollinear magnetism and corresponding spin spiral chirality through interlayer sliding. Our work provides another perspective for the development of magnetoelectric physics and information storage devices.

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