Large-area fast lithium ion conducting ceramic thin freestanding sheets was successfully prepared using a sheet forming technique. This ceramic sheet contains the crystalline phase of Li1+x+yAlxTi2-xSiyP3-yO12 with the NASICON type structure. The ceramic sheet showed maximum overall conductivity over 10−3 S cm−1 at room temperature. And, the developed thin ceramic sheet has sufficient flexibility against bending stress. Because a thin large-area ceramic electrolyte sheet was prepared using less energy compared with a conventional glass casting method, it is suitable for practical use.