Abstract: A series of hydrotalcite-like Ti/Li/Al-LDHs materials were prepared by co-precipitation method and characterized by atomic absorption spectrophotometer (AAS), X-ray diffraction (XRD), scanning electron microscopy (SEM), thermal gravimetric analysis (TG) and Fourier transform infrared (FT-IR); the influence of metal composition and calcination temperature on the structure, morphology and CO₂ adsorption capacity of Ti/Li/Al-LDHs was investigated. The results showed that Ti₁Li₃Al₄-LDHs obtained with a Ti/Li/Al ratio of 1:3:4 displays the highest crystallinity and regular morphology, whereas Ti₁Li₃Al₂-LDHs₃₀₀ prepared with a Ti/Li/Al ratio of 1:3:2 and calcined at 300℃ exhibits the best adsorption performance towards CO₂. The CO₂ adsorption capacity over Ti₁Li₃Al₂-LDHs₃₀₀ reaches 53.5mg/g; in addition, the adsorption capacity is only decreased by 2.4% after adsorption for 10 cycles.