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The application discloses high-quality bismuth-based perovskite monocrystals and a preparation method and application thereof. The preparation method of the high-quality bismuth-based perovskite monocrystals comprises the following steps: S1, preparing a single crystal growth precursor solution of the bismuth-based perovskite; S2, performing heat aging treatment on the prepared single crystal growth precursor solution; and S3, controlling the single crystal growth precursor solution after the heat aging treatment to crystallize and grow the bismuth-based perovskite monocrystals. The heat aging process of the precursor solution can obviously reduce the nucleation rate, effectively improve the crystallization quality, and finally obtain large-size high-quality bismuth-based perovskite monocrystals. The method has the advantages of simple process, strong operability, mild growth conditions, low required temperature, energy saving, low equipment requirement, low cost, high success rate, no need of additional seed crystals, and continuous growth of large-size high-quality perovskite monocrystals.