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The bismuth layer-structured ferroelectrics (BLSFs) materials have potential for high-temperature piezoelectric applications. Among these piezoelectric materials, the CaBi₄Ti₄O₁₅ (CBT) piezoelectric ceramic with a high decomposition temperature of about 1250 °C attracts a lot of attention. Achieving a CBT single crystal is a significant way to improve its piezoelectric properties. For this purpose, the flux system for growing CBT crystal was explored in this study. The optimum flux composition ratio was found to be PbO:B₂O₃:CBT = 3:3:1 in mol%, where the PbO–B₂O₃ mixtures were used as a flux system. Millimeter size flake-shaped CBT crystals were obtained using the spontaneous growth process for the first time. The relationship between the crystal structure and flake growth habit was analyzed. In addition, the bandgap was evaluated by the combination of transmittance spectrum and first-principle calculations. Besides, the piezoelectric property was predicted from the perspective of polyhedral distortion, which indicated the potential of CBT crystal for piezoelectric applications.