LAUSR

Polarization‐sensitive photodetectors based on anisotropic semiconductors sense both the intensity and polarization state information without extra optical components. Here, a self‐powered organic photodetector (OPD) composed of intrinsically stretchable polymer donor PNTB6‐Cl and non‐fullerene acceptor Y6 is reported. The PNTB6‐Cl:Y6 photoactive film accommodates a remarkable 100% strain without fracture, exhibiting a high optical anisotropy of 1.8 after strain alignment. The resulting OPD not only shows an impressive faint‐light detection capability (high spectral responsivity of 0.45 A W−1 and high specific detectivity of 1012 Jones), but also has a high anisotropic responsivity ratio of 1.42 under the illumination of parallel and traversed polarized light. To the best of the authors’ knowledge, both the detector performance and polarization features are among the best‐performing OPDs and polarization‐sensitive photodetectors. As a proof‐of‐concept, polarization‐sensitive OPDs are also utilized to set up a polarimetric imaging system and full‐Stokes polarimeter. This work explores the potential of highly stretchable organic semiconductors for state‐of‐art polarization imaging and spectroscopy applications.