Strain Engineering of Magnetoresistance and Magnetic Anisotropy in CrSBr

Abstract Tailoring magnetoresistance and magnetic anisotropy in van der Waals magnetic materials is essential for advancing their integration into technological applications. In this regard, strain engineering has emerged as a powerful and versatile strategy to control magnetism at the 2D limit. Here, it is demonstrated that compressive biaxial strain significantly enhances the magnetoresistance and magnetic anisotropy of few‐layer CrSBr flakes. Strain is efficiently transferred to the flakes from the thermal compression of a polymeric substrate upon cooling, as confirmed by temperature‐dependent Raman spectroscopy. This strain induces a remarkable increase in the magnetoresistance ratio and in the saturation fields required to align the magnetization of CrSBr along each of its three crystalographic directions, reaching a twofold enhancement along the magnetic easy axis. This enhancement is accompanied by a subtle reduction of the Néel temperature by ≈10 K. The experimental results are fully supported by first‐principles calculations, which link the observed effects to a strain‐driven modification in interlayer exchange coupling and magnetic anisotropy energy. These findings establish strain engineering as a key tool for fine‐tuning magnetotransport properties in 2D magnetic semiconductors, paving the way for implementation in spintronics and information storage devices.