The glycol solvent -thermal method prepared a serial of NiAlNd catalysts based on layered double hydrox-ides (LDHs) precursor. The introduction of Nd greatly promoted the catalytic activity for CO₂ methanation at low temperatures. The CO₂ conversion on the NiAlNd - 0.4 catalyst reached 83.9% under the reaction condition: T= 210 ℃, WHSV (weight hourly space velocity)=24 000 mL·g^-1·h^-1, p=100 kPa. The substitution of Nd³⁺ for Al³⁺ hin-dered the formation of LDHs structure in the precursor but decreased the particle size of the calcined catalyst. The interaction between NiO and Al₂O₃ was weakened with the introduction of Nd, resulting in better NiO component reducibility and high intrinsic activity of the Ni site. Moreover, the presence of Nd increased the number of surface basic sites of the catalyst, thus increasing the adsorption of CO₂. With the increase in Nd, the surface area of metallic Ni in the reduced catalyst takes on a volcano-shape variation trend. The catalytic activities of NiAlNd catalysts are affected by the number and intrinsic activity of Ni sites simultaneously.