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Highlights: A flexible tribotronic artificial synapse with bioinspired neurosensory behaviour was demonstrated, which establishes an active interaction mechanism with the environment. The device can well exhibit tuneable synaptic behaviours by changing the mechanical input modes, including excitatory postsynaptic current, paired-pulse facilitation, and the hierarchical memorial process. The device has excellent mechanical flexibility that can exhibit stable synaptic functions even under strain conditions with a bending radius of 20 mm after 1000 bending cycles. As key components of artificial afferent nervous systems, synaptic devices can mimic the physiological synaptic behaviors, which have attracted extensive attentions. Here, a flexible tribotronic artificial synapse (TAS) with bioinspired neurosensory behavior is developed. The triboelectric potential generated by the external contact electrification is used as the ion-gel-gate voltage of the organic thin film transistor, which can tune the carriers transport through the migration/accumulation of ions. The TAS successfully demonstrates a series of synaptic behaviors by external stimuli, such as excitatory postsynaptic current, paired-pulse facilitation, and the hierarchical memory process from sensory memory to short-term memory and long-term memory. Moreover, the synaptic behaviors remained stable under the strain condition with a bending radius of 20 mm, and the TAS still exhibits excellent durability after 1000 bending cycles. Finally, Pavlovian conditioning has been successfully mimicked by applying force and vibration as food and bell, respectively. This work demonstrates a bioinspired flexible artificial synapse that will help to facilitate the development of artificial afferent nervous systems, which is great significance to the practical application of artificial limbs, robotics, and bionics in future. [ABSTRACT FROM AUTHOR]