Being able to probe the polarization states of light is crucial for applications from medical diagnostics and bio-inspired navigation to information encryption and quantum computing. Current state-of-the-art polarimeters based on anisotropic semiconductors enable direct linear dichroism photodetection without the need for bulky and complex external optics. However, their polarization sensitivity is restricted by the inherent optical anisotropy, leading to low dichroic ratios of typically smaller than ten. Here, we unveil an effective and general design rule to achieve a more than 2,000-fold enhanced polarization sensitivity by exploiting a light-induced anisotropic gating effect in organic phototransistors. The polarization-dependent trapping of photogenerated charge carriers provides an anisotropic photo-induced gate for current amplification, which has resulted in an extremely high dichroic ratio of over 1.2×104, more than two orders of magnitude higher than any previous reports. These findings further enable the first demonstration of a novel miniaturized bionic celestial compass for skylight-based polarization navigation. Our results offer a fundamental design principle and a new route for the development of next-generation highly polarization-sensitive optoelectronics.