AbstractOptoelectronic synapses with information sensing, processing, and memory function are promoting the development of artificial visual perception systems. However, optoelectronic synapses' relatively inferior optoelectronic performance impedes their application in complex neuromorphic computing. Herein, optoelectronic synapses based on 3D graphene/molybdenum disulfide (MoS2) heterostructure field‐effect transistors are developed by using the double stress layer self‐rolled‐up method. The graphene, with excellent electrical properties, enhances the carrier transport capacity of the device. The unique continuous photoconductivity of MoS2 is suitable for simulating various synaptic nerve morphological functions. Meanwhile, the 3D resonant microcavity is added to enhance the optical field and make the device polarization sensitive, which reveals more intangible features of objects. The device demonstrates room‐temperature photodetection at ultraviolet, visible, near‐infrared, and mid‐infrared regions, with photoresponsivity up to 105 A W−1 at 590 nm. Furthermore, multiple synaptic neuromorphic functions, such as inhibitory postsynaptic current, paired‐pulse facilitation, short‐term depression, and long‐term depression, are successfully emulated. Here a new concept is provided for designing high‐performance optoelectronic synapses with polarization sensitivity and excellent potential in artificial intelligence is shown.