A novel alkaline hydrothermal approach for low-temperature conversion of α-spodumene into Li 2 SiO 3 residue was proposed, providing a promising method for extracting lithium from α-spodumene as a pretreatment process. This work proposed a systematic investigation for extracting lithium from the residue by acid leaching and preparing lithium carbonate. The reaction feasibility between Li 2 SiO 3 and acids (HCl and H 2 SO 4 ) was first evaluated through thermodynamic calculation. Compared with the leaching effects of hydrochloric acid and sulphuric acid, sulphuric acid is the preferred leaching agent due to its higher extraction efficiency for lithium and lower acid consumption. Lithium extraction efficiency from the residue achieved up to 87.48% under the following optimized conditions: 0.75 mol/L H 2 SO 4 , 0.4 times the theoretical amount of acid, 10 min, 30 C, and 100 rpm. Based on the optimized conditions, the lithium-