Optical anisotropy plays an indispensable role in a variety of optical components. Organic halide perovskites often rely on artificially oriented nanostructures to enhance optical anisotropy due to their in-plane isotropic crystal structure, which results in unnecessary optical losses and fabrication difficulties. Here, we report the large optical anisotropy in two-dimensional perovskite [CH(NH2)2][C(NH2)3]PbI4 crystals. Without specially designing their morphology, we achieved a large photoresponse linear dichroic ratio of 2 and a photoluminescence linear dichroic ratio of 4.7. Furthermore, we identified that the polarization orientation is parallel to the corrugated inorganic layers on every crystal plane by density functional theory calculations. The anisotropy of the ab-plane and ac-plane changes in opposite trend with temperature, suggesting that the perovskite can selectively generate polarized light or unpolarized light from different crystal planes by tuning the temperature. Our studies provide a new platform toward two-dimensional perovskite-based optical polarization devices.