LAUSR

Organic semiconductors have demonstrated exceptional performance due to their inherent advantages such as simple processability, and superior mechanical properties. Developing polarization‐sensitive near‐infrared (NIR) organic photodetectors is crucial for their application in target recognition, biological imaging, and wearable optoelectronics. However, high‐performance NIR photon detection still faces challenges for organic materials, due to their intrinsic limitations including low carrier mobility, and poor exciton dissociation. Here, a polarization‐sensitive NIR photodetector is demonstrated with a linear dichroic ratio of 5.3, employing a two‐dimensional (2D) TiOPc single‐crystal/graphene heterostructure. Remarkable absorption, optimized exciton diffusion of single crystal, and efficient interfacial charge transfer enable a high NIR responsivity of > 103 A W−1 and specific detectivity of 1010 Jones for 980 nm irradiation, with a reasonable −3 dB bandwidth of >1 kHz. Under 850 nm illumination, it exhibits an even higher responsivity of > 104 A W−1 and specific detectivity of > 1011 Jones, attributed to stronger absorption. This NIR responsivity represents a tenfold improvement over existing organic polarization photodetectors. Finally, the high‐resolution polarization‐dependent single‐pixel imaging in NIR range is achieved, highlighting its great potential for image recognition applications. This work opens new avenues for exploiting high‐performance NIR polarized photodetectors.