The non-centrosymmetric bismuth-based oxyborate crystals have been extensively studied for non-linear optical, opto-electric and piezoelectric applications. In this work, single crystal growth and electro-elastic properties of α-BiB 3 O 6 (α-BIBO) and Bi 2 ZnB 2 O 7 (BZBO) crystals are reported. Centimeter-sized α-BIBO and BZBO crystals were grown by using the Kyropoulos method. High resolution X-ray diffraction tests were performed to assess the crystal quality. The full-width at half-maximum values (FWHM) of the rocking curves were evaluated to be 35.35 arcsec and 47.85 arcsec for α-BIBO and BZBO samples, respectively. Moreover, the electro-elastic properties of α-BIBO and BZBO crystals are discussed and summarized, based on which the radial extensional and the face shear vibration modes were studied for potential acoustic device applications. The radial extensional mode electro-mechanical coupling factors k p were evaluated and found to be 32.0% and 5.5% for α-BIBO and BZBO crystals, respectively. The optimal crystal cuts with face shear mode were designed and found to be (YZt)/−53 • (or (YZt)/37 • cut) for α-BIBO crystal, and (ZXt)/±45 • cut for BZBO crystal, with the largest effective piezoelectric coefficients being in the order of 14.8 pC/N and 8.9 pC/N, respectively.