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It is urgent to reduce the emission of carbon dioxide (CO2) into the atmosphere and thereby mitigate climate changes. To implement the industrial scenario of carbon capture and storage (CCS), there is a great need for the discovery or development of excellent solid CO2 sorbents with technological and economic feasibility. Lithium orthosilicate (Li4SiO4) has been identified as one of the most promising candidates for CO2 capture at high temperatures and has drawn worldwide research interests. In the last years, focusing on the ultimate goal of achieving a Li4SiO4 sorbent with excellent physicochemical performance for various industrial applications, extensive works have been conducted, including exploring suitable preparation methods, modeling analysis, various modifications for performance enhancement, optimization of operation conditions, granulation and their applications. This work summarizes the state-of-the-art researches in the literature aiming at developments of Li4SiO4 sorbents for high-temperature CO2 capture. The potential new development trends are also discussed in the current work.