Thermochemical energy storage (TCES) is one of the key technologies facilitating the integration of renewable energy sources and mitigating the climate crisis. Recently, Li
4SiO
4 has been reported to be a promising heat carrier material for TCES applications, owing to its moderate operation temperature and stability. During the synthetic processes, the properties of the Si source used directly influence the performance of derived Li
4SiO
4 materials; however, the internal relations and effects are not yet clear. Hence, in this work, six kinds of SiO
2 sources with different phases, morphology, particle size, and surface area were selected to synthesize a Li
4SiO
4-based TCES heat carrier. The physicochemical properties of the SiO
2 and the corresponding derived Li
4SiO
4 were characterized, and the comprehensive performance (e.g., heat storage/releasing capacity, rate, and cyclic stability) of the Li
4SiO
4 samples was systematically tested. It was found that the silica microspheres (SPs), which possess an amorphous phase, uniform micro-scale structure, and small particle size, could generate Li
4SiO
4 TCES materials with a highest initial capacity of 777.7 kJ/kg at 720 °C/900 °C under pure CO
2. As a result, the SP-L showed an excellent cumulative heat storage amount of 5.84 MJ/kg within 10 heat-releasing/storage cycles, which was nearly 1.5 times greater than the value of Li
4SiO
4 derived from commonly used silicon dioxide. Furthermore, the effects of the utilized Si source on the performance of as-prepared Li
4SiO
4 and corresponding mechanisms were discussed, which offers guidance for the future selection of Si sources to produce high-performance Li
4SiO
4-based TCES heat carriers.
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