AbstractIntelligent wearable devices are essential for telemedicine healthcare as they enable real‐time monitoring of physiological information. Elaborately constructing synapse‐inspired materials provides a crucial guidance for designing high‐performance sensors toward multiplex stimuli response. However, a realistic mimesis both in the “structure and sense” of biological synapses to obtain advanced multi‐functions is still challenging but essential for simplifying subsequent circuit and logic programs. Herein, an ionic artificial synapse integrated with Ti3CNTxnanosheets in situ grown with zeolitic imidazolate framework flowers (ZIF‐L@Ti3CNTxcomposite) is constructed to concurrently mimic the structure and working mechanism of the synapse. The flexible sensor of the bio‐inspired ZIF‐L@Ti3CNTxcomposite exhibits excellent dual‐mode dimethylamine (DMA) and strain‐sensitive response with non‐overlapping resistance variations. The specific ions conduction working principle triggered by DMA gas or strain with the assistance of humidity is confirmed by the density functional theory simulation. Last, an intelligent wearable system is self‐developed by integrating the dual‐mode sensor into flexible printed circuits. This device is successfully applied in pluralistic monitoring of abnormal physiological signals of Parkinson's sufferers, including real‐time and accurate assessment of simulated DMA expiration and kinematic tremor signals. This work provides a feasible routine to develop intelligent multifunctional devices for upsurging telemedicine diagnosis.