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Two-dimensional (2D) multiferroics that simultaneously host ferroelectricity and magnetism represent a frontier platform for next-generation electronics and spintronics. Here we demonstrate that Cr2S3 thin film serves as a rare intrinsic room-temperature sliding multiferroic with coexisting ferroelectric, ferromagnetic, and ferrovalley orders. Crucially, interlayer sliding drives reversible ferroelectric polarization switching, resulting in a stabilized ferroelectricity with a critical temperature TFE ~ 420 K. Furthermore, the system exhibits robust perpendicular magnetic anisotropy with intralayer and interlayer ferromagnetic coupling (TFM ~ 300 K), sharply contrasting with the prevalent interlayer A-type antiferromagnetism in conventional sliding ferroelectrics. Remarkably, an electric field is able to achieve linear magnetoelectric coupling in Cr2S3 to realize electronic control of magnetism. Fundamental symmetry breaking further generates giant spontaneous valley polarization, while the antisymmetric Berry curvature mediates electrically programmable anomalous valley Hall effect. This functional integration establishes a multipath quantum control where interlayer sliding, spin orientation, and valley pseudospin are strongly coupled. This work opens routes to room-temperature atomically-scaled multistate devices, including nonvolatile memories, magnetoelectric sensors, and valleytronic logic devices.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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