3D perovskite CsPbBr3 has recently taken a blooming position for optoelectronic applications. However, due to the lack of natural anisotropy of optical attributes, it is a great challenge to fulfil polarization‐sensitive photodetection. Here, for the first time, we exploited dimensionality reduction of CsPbBr3 to tailor a 2D‐multilayered hybrid perovskite, (TRA)2CsPb2Br7 (1, in which TRA is (carboxy)cyclohexylmethylammonium), serving as a potential polarized‐light detecting candidate. Its unique quantum‐confined 2D structure results in intrinsic anisotropy of electrical conductivity, optical absorbance, and polarization‐dependent responses. Particularly, it exhibits remarkable dichroism with the photocurrent ratio (Ipc/Ipa) of ≈2.1, being much higher than that of the isotropic CsPbBr3 crystal and reported CH3NH3PbI3 nanowire (≈1.3), which reveals its great potentials for polarization‐sensitive photodetection. Further, crystal‐based detectors of 1 show fascinating responses to the polarized light, including high detectivity (>1010 Jones), fast responding time (≈300 μs), and sizeable on/off current ratios (>104). To our best knowledge, this is the first study on 2D Cs‐based hybrid perovskite exhibiting strong polarization‐sensitivity. The work highlights an effective pathway to explore new polarization sensitive candidates for hybrid perovskites and promotes their future electronic applications.