Abstract: | Polarization‐sensitive photodetection in the UV region is highly indispensable in many military and civilian applications. UV‐polarized photodetection usually relies on the use of wide bandgap semiconductors with 1D nanostructures requiring complicated nanofabrication processes. Although the emerging anisotropic 2D semiconductors shed light on the detection of polarization with a simple device architecture, bandgaps of such reported 2D semiconductors are too small to be applied for visible–blind UV‐polarized photodetection. Here, germanium disulfide (GeS2), the widest bandgap (>3 eV) in the family of in‐plane anisotropic 2D semiconductors explored to date, is introduced as an ideal candidate for UV‐polarized photodetection. The structural, vibrational, and optical anisotropies of GeS2 are systematically investigated from theory to experiment. GeS2‐based photodetectors show a strong polarization‐dependent photoresponse in the UV region. GeS2 with a wide bandgap and high in‐plane anisotropy not only enriches the family of anisotropic 2D semiconductors but also expands the polarized photodetection from the current visible and near‐infrared to the brand‐new UV region. |