Artificial multisensory devices play a key role in human-computer interaction in the field of artificial intelligence (AI). In this work, we have designed and constructed a novel olfactory-visual bimodal neuromorphic carbon nanotube thin film transistor (TFT) arrays for artificial olfactory-visual multisensory synergy recognition with a very low power consumption of 25 aJ for a single pulse, employing semiconducting single-walled carbon nanotubes (sc-SWCNTs) as channel materials and gas sensitive materials, and poly[[4,8-bis[5-(2-ethylhexyl)-2-thienyl]benzo[1,2-b:4,5-b0]dithiophene-2,6-diyl]-2,5-thiophenediyl-[5,7-bis(2-ethylhexyl)-4,8-dioxo-4H,8H-benzo[1,2-c:4,5-c0]dithio-phene-1,3-diyl]] (PBDB-T) as the photosensitive material. It is noted that it is the first time to realize the simulation of olfactory and visual senses (from 280 nm to 650 nm) with the wide operating temperature range (0–150 °C) in a single SWCNT TFT device and successfully simulate the recovery of olfactory senses after COVID-19 by olfactory-visual synergy. Furthermore, our SWCNT neuromorphic TFT devices with a high I_On/I_Off ratio (up to 10⁶) at a low operating voltage (−2 to 0.5 V) can mimic not only the basic biological synaptic functions of olfaction and vision (such as paired-pulse facilitation, short-term plasticity, and long-term plasticity), but also optical wireless communication by Morse code. The proposed multisensory, broadband light-responsive, low-power synaptic devices provide great potential for developing AI robots to face complex external environments.