Centimeter-sized Ca₂Nb₂O₇ crystals were successfully grown using the conventional Czochralski pulling method with an optimized crystal growth technique. Single-crystal X-ray diffraction studies indicated that the Ca₂Nb₂O₇ crystal belongs to the Pna2₁ space group with orthorhombic symmetry. The unit cell parameters were determined to be a = 26.471 Å, b = 7.688 Å, and c = 5.490 Å, while the thermal expansion coefficients were measured to be α₁₁ = 5.83, α₂₂ = 7.94, and α₃₃ = 13.32 (10⁻⁶ °C⁻¹). In addition, the ferroelectric properties of the crystal were also determined (i.e., P_r = 5.62 μC cm⁻¹, E_c = 99.1 kV cm⁻¹). Furthermore, simultaneous thermal analysis showed that the ferroelectric phase exists stably even when the temperature rises to 1400 °C. The full set of electro-elastic constants for the Ca₂Nb₂O₇ crystal were determined by the resonance method, wherein the piezoelectric coefficient d₃₃ was 8.5 pC N⁻¹ and the electromechanical coupling factor k₃₃ was 20.4%. As a ferroelectric crystal with a high Curie temperature, Ca₂Nb₂O₇ exhibits a high piezoelectric coefficient, a high electromechanical coupling coefficient, and excellent potential for use in high-temperature piezoelectric sensing applications.