Polarized-light detection in solar-blind ultraviolet region is indispensable for optoelectronic applications,whereas new 2D candidates targeted at solar-blind UV range remain extremely scarce.2 Dh ybrid perovskite ferroelectrics that combine polarization and semiconducting properties are of increasing interest. Here,u sing the 3D-to-2D dimensional reduction of CH 3 NH 3 PbCl 3 ,wedesigned amultilayered hybrid perovskite ferroelectric,(CH 3 CH 2 NH 3) 2 (CH 3 NH 3) 2 Pb 3 Cl 10 , which shows spontaneous polarization and ah igh Curie temperature (390 K) comparable with that of BaTiO 3 (393 K). The wide band gap (ca. 3.35 eV) and anisotropic absorbance stemming from its intrinsic 2D motif,greatly favor its polarization-sensitive activity in UV region. The device displays excellent polarization-sensitive behavior under 266 nm, along with al arge dichroic ratio (ca. 1.38) and high on/off current ratio (ca. 2.3 10 3).