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An ultrasensitive methanol gas sensing device based on the quasi-molecular imprinting technology (quasi-MIT) is studied in this work. We applied the sol-gel method (ALS denotes Ag-LaFeO
3
prepared by the sol-gel method) and combustion synthesis (ALC denotes Ag-LaFeO
3
prepared by combustion synthesis) to prepare Ag-LaFeO
3
based sensors. The morphologies and structures of the Ag-LaFeO
3
materials were examined via various detection techniques. The ALSM and ALCM sensor (ALSM and ALCM denotes the devices prepared by coating the ALS and ALC materials with methanol, respectively) fabricated using the sol-gel method and combustion synthesis combined with quasi-MIT exhibit good gas sensing properties to methanol, in contrast with the two devices (ALSW and ALCW denote the devices prepared for coating the ALS and ALC materials with water, respectively) without the use of quasi-MIT. The results show that quasi-MIT introduced the target gas in the fabrication process of the device, playing an important role in the design of the ultrasensitive methanol gas sensor. The sensing response and the optimum working temperature of ALSM and ALCM gas sensor are 52.29 and 155 °C and 34.89 and 155 °C, respectively, for 5 ppm methanol, and the highest response to other gases is 8. The ALSM and ALCM gas sensors reveal good selectivity and response for methanol.