2D layered materials with sensitive surfaces are promising materials for use in chemical sensing devices, owing to their extremely large surface‐to‐volume ratios. However, most chemical sensors based on 2D materials are used in the form of laterally defined active channels, in which the active area is limited to the actual device dimensions. Therefore, a novel approach for fabricating self‐formed active‐channel devices is proposed based on 2D semiconductor materials with very large surface areas, and their potential gas sensing ability is examined. First, the vertical growth phenomenon of SnS2 nanocrystals is investigated with large surface area via metal‐assisted growth using prepatterned metal electrodes, and then self‐formed active‐channel devices are suggested without additional pattering through the selective synthesis of SnS2 nanosheets on prepatterned metal electrodes. The self‐formed active‐channel device exhibits extremely high response values (>2000% at 10 ppm) for NO2 along with excellent NO2 selectivity. Moreover, the NO2 gas response of the gas sensing device with vertically self‐formed SnS2 nanosheets is more than two orders of magnitude higher than that of a similar exfoliated SnS2‐based device. These results indicate that the facile device fabrication method would be applicable to various systems in which surface area plays an important role. A novel approach for fabricating self‐formed active‐channel devices based on 2D semiconductor materials with very large surface areas is proposed and their potential gas sensing ability is examined. The device exhibits extremely high response values and this novel fabrication method is expected to find use in various applications where surface area plays an important role in function.