BackgroundCO2 emissions have had negative impacts on various aspects of life and the environment, making the development of materials with high CO2 adsorption performance crucial.ResultIn this study, halloysite nanotubes (HNTs) were used as a carrier to prepare MgAl layered double hydroxide (LDH) via a convenient coprecipitation method, resulting in MgAl‐LDH/HNT composite material, which was then evaluated for its CO2 adsorption performance. The physicochemical properties of the composite material were characterized using various methods. Results showed that the 1:1 ratio MgAl‐LDH/HNT composite exhibited superior material structure, with a specific surface area reaching 178.24 m2 g−1. In CO2 adsorption performance tests, the 1:1 MgAl‐LDH/HNT composite showed the best adsorption performance, with a CO2 adsorption capacity of 3.91 mmol g−1. This adsorption process includes physical adsorption and chemical adsorption. Kinetic analysis results indicate that the adsorption process is mainly dominated by physical adsorption. The material also demonstrated good performance in cyclic stability tests, maintaining a regeneration efficiency of over 94% after six cycles.ConclusionThe MgAl‐LDH/HNT material has good properties and stability. This provides an effective pathway and direction for the development of new adsorbents with higher CO2 adsorption performance. © 2024 Society of Chemical Industry (SCI).