Abstract2D van der Waals heterojunctions (vdWH) have emerged as an attractive platform for the realization of optoelectronic synaptic devices, which are critical for energy‐efficient computing systems. Photogating induced by charge traps at the interfaces indeed results in ultrahigh responsivity and tunable photoconductance. Yet, optical potentiation and depression remain mostly modulated by gate bias, requiring relatively high energy inputs. Thus, advanced all‐optical synapse switching strategies are still needed. In this work, a reversible switching between positive photoconductivity (PPC) and negative photoconductivity (NPC) is achieved in graphene/WSe2 vdWH solely through light‐intensity modulation. Consequently, the graphene/WSe2 synaptic device shows tunable optical potentiation and depression behavior with an ultralow power consumption of 127 aJ. The study further unravels the complex interplay of gate bias and incident light power in determining the sign and magnitude of the photocurrent, showing the critical role of charge trapping and photogating at interfaces. Interestingly, it is found that switching between PPC to NPC can be also obtained at 0 mV drain‐source voltage. Overall, the reversible potentiation/depression effect based on light intensity modulation and its combination with additional gate bias tunability is very appealing for the development of energy‐efficient optical communications and neuromorphic computing.