BaTiO3 (BTO) ferroelectric films, which are renowned for their lead-free compositions, superior stability, and absence of a wake-up effect, are promising candidate materials in the field of non-volatile memories. However, the prerequisites for high-temperature conditions in the fabrication of ferroelectric thin films impose constraints on the substrate choice, which has limited the advancement in non-volatile memories based on single-crystal flexible BTO films with robust ferroelectric properties. Herein, a technique has been developed for the fabrication of flexible devices using a pulsed laser deposition system. BTO ferroelectric films have then been deposited onto a flexible mica substrate, with SrTiO3 (STO) serving as a buffer layer. The obtained flexible BTO devices exhibited excellent ferroelectricity, with a maximum polarization (2Pmax) of up to 42.58 μC/cm2 and a remnant polarization (2Pr) of up to 21.39 μC/cm2. Furthermore, even after 1000 bending cycles, the bipolar switching endurance remained high at 1012 cycles. After 104 s, the flexible BTO device still maintained excellent polarization characteristics. These results make the flexible BTO ferroelectric thin film a potential candidate for the next generation of non-volatile memories.