Nitrogen oxides are one of the main atmospheric pollutants and pose a threat to the ecological environment and human health. Selective catalytic reduction (NH3-SCR) is an effective way of removing nitrogen oxides, with the catalyst being the key to this technology. Two-dimensional nanostructured layered double oxide (LDO) has attracted increasing attention due to the controllability of cations in the layers and the exchangeability of anions between layers. As a derivative of layered double hydroxide (LDH), LDO not only inherits the controllability and diversity inherent in the LDH structure but also exhibits excellent performance in the catalytic field. This article contains three main sections. It begins with a brief discussion of the development of LDO catalysts and analyzes the advantages of the LDO structure. The later section introduces the synthesis methods of LDH, clarifies the conversion relationship between LDH and LDO, and summarizes the modification impacts of the properties of LDO catalysts. The application of LDO catalysts used in NH3-SCR under wild temperature conditions is discussed, and the different types, reaction processes, and mechanisms of LDO catalysts are described in the third section. Finally, future research directions and outlooks are also offered to assist the development of LDO catalysts and overcome the difficult points related to NH3-SCR.