“…Low‐symmetry 2D materials with intrinsic in‐plane anisotropy have become a major research direction in 2D field because of their applications in next‐generation anisotropic multifunctional devices, e.g., polarization‐sensitive photodetectors, linearly polarized pulse generators, high‐gain digital inverters, and anisotropic memorizers. [ 1–3 ] Currently, only several in‐plane anisotropic 2D materials have been discovered, including black phosphorous (BP), [ 4 ] 1Td WTe 2 , [ 5 ] GeSe 2 , [ 6 ] GeP, [ 7 ] GaTe, [ 8 ] ReQ 2 (Q = S, Se), [ 9,10 ] Ta 2 NiS 5 , [ 11 ] and TaIrTe 4 , [ 12 ] and so on. However, most of them have drawbacks in anisotropic device application, such as poor stability (few‐layer BP, [ 4 ] 1Td WTe 2 , [ 13 ] GeSe 2 , [ 6 ] GeP, [ 7 ] and GaTe [ 8 ] ), low anisotropic ratios (ReQ 2 [ 9,10 ] and Ta 2 NiS 5 [ 11 ] ), and low current on/off ratio (TaIrTe 4 [ 14 ] ), greatly restricting their applications in anisotropic optics, electronics, and optoelectronics.…”