We demonstrate a highly selective and reversible NO 2 resistive gas sensor using vertically aligned MoS 2 (VA-MoS 2 ) flake networks. We synthesized horizontally and vertically aligned MoS 2 flakes on SiO 2 /Si substrate using a kinetically controlled rapid growth CVD process. Uniformly interconnected MoS 2 flakes and their orientation were confirmed by scanning electron microscopy, x-ray diffraction, Raman spectroscopy and x-ray photoelectron spectroscopy. The VA-MoS 2 gas sensor showed two times higher response to NO 2 compared to horizontally aligned MoS 2 at room temperature. Moreover, the sensors exhibited a dramatically improved complete recovery upon NO 2 exposure at its low optimum operating temperatures (100 °C). In addition, the sensing performance of the sensors was investigated with exposure to various gases such as NH 3 , CO 2 , H 2 , CH 4 and H 2 S. It was observed that high response to gas directly correlates with the strong interaction of gas molecules on edge sites of the VA-MoS 2 . The VA-MoS 2 gas sensor exhibited high response with good reversibility and selectivity towards NO 2 as a result of the high aspect ratio as well as high adsorption energy on exposed edge sites.