Multiferroics exhibiting simultaneous magnetic and ferroelectric orders constitute essential systems for realizing magnetoelectric coupling, thereby presenting considerable promise for technological applications. However, the development of multiferroics faces a persistent challenge: achieving the coexistence of robust magnetoelectric coupling and pronounced ferroelectric polarization. In this study, we demonstrate the emergence of spin-driven ferroelectricity in $\mathrm{C}{\mathrm{r}}_2{\mathrm{S}}_3$ through first-principles calculations. The system exhibits out-of-plane polarization significantly exceeding that of most conventional type-II multiferroics, and features a unique pathway for ferroelectric switching through spin rotation. Furthermore, two-dimensional $\mathrm{C}{\mathrm{r}}_2{\mathrm{S}}_3$ demonstrates half-metallic behavior and maintains spin-induced ferroelectric polarization. This discovery marks a substantial advancement in the design of multiferroics.

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• Ferroelectrics
• Multiferroics
• Ferrimagnets
• Density functional theory