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Highlights The photoelectric response of violet phosphorus (VP) is significantly enhanced by the MXene/VP van der Waals heterojunctions and the highest photoresponsivity of VP is demonstrated. The first VP-based optoelectronic synapse with essential synaptic behaviours is demonstrated. Proof-of-concept visual-olfactory crossmodal perception based on MXene/VP optoelectronic synapses is explored to mimic neuromorphic vision with multi-sensory interactions.