Antimony triselenide (Sb 2 Se 3 ) nanoflake-based nitrogen dioxide (NO 2 ) sensors exhibit a progressive bifunctional gas-sensing performance, with a rapid alarm for hazardous highly concentrated gases, and an advanced memory-type function for low-concentration (<1 ppm) monitoring repeated under potentially fatal exposure. Rectangular and cuboid shaped Sb 2 Se 3 nanoflakes, comprising van der Waals planes with large surface areas and covalent bond planes with small areas, can rapidly detect a wide range of NO 2 gas concentrations from 0.1 to 100 ppm. These Sb 2 Se 3 nanoflakes are found to be suitable for physisorption-based gas sensing owing to their anisotropic quasi-2D crystal structure with extremely enlarged van der Waals planes, where they are humidity-insensitive and consequently exhibit an extremely stable baseline current. The Sb 2 Se 3 nanoflake sensor exhibits a room-temperature/low-voltage operation, which is noticeable owing to its low energy consumption and rapid response even under a NO 2 gas flow of only 1 ppm. As a result, the Sb 2 Se 3 nanoflake sensor is suitable for the development of a rapid alarm system. Furthermore, the persistent gassensing conductivity of the sensor with a slow decaying current can enable the development of a progressive memory-type sensor that retains the previous signal under irregular gas injection at low concentrations.