In recent years, the unique properties of Layered Double Hydroxides (LDHs) led to an interest in using LDHs as sensors, but gas sensing properties of LDHs have not still been broadly investigated. In this work, Ni-Cr-Al LDH was synthesized by co-precipitation method and was characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and Fourier-transform infrared spectroscopy (FTIR), and then, its sensing properties were investigated in the presence of various gases at room temperature (25 ± 2 °C). It was observed that the sensors resistance changes in the presence of acetone were descending, and the opposite trend was observed for alcohols. The sensor's selectivity and stability were acceptable, but its response and recovery times were somewhat long (about a few minutes).