Gangqiang Zhou, Jiyuan Xu, Zimeng Wang, Nitin Mallik, Azzedine Bendounan, Zailan Zhang, Zhesheng Chen
ABSTRACT The stacking of different 2D materials provides an extraordinary platform for multifunctional optoelectronic devices. However, for 2D anisotropic materials, which offer an additional degree of freedom for controlling in‐plane photoelectric performance, their stacking for multifunctional device applications remains limited. Here, as an example, we fabricated an anisotropic PdSe 2 /GeAs heterojunction and achieved multifunctional operations. First, the device exhibits self‐driven performance with a responsivity of up to 680 mA/W, a detectivity of 1.1 × 10 11 Jones, and an external quantum efficiency as high as 158%. In addition, the device demonstrates excellent capabilities in high‐resolution polarization imaging and image convolution processing. Furthermore, the polarity of photocurrent in the device can be switched as a function of gate voltage. By combining multi‐modal control strategies through both electrical and optical regulation, the device achieves multi‐state logic outputs and programmable photonic logic gate functions. This work provides new insights into the development of highly integrated and multifunctional optoelectronic systems based on anisotropic heterostructures, paving the way toward intelligent optical sensing and high‐speed optical communication applications.