A full set of acoustical physical constants was determined for Ca 3 TaGa 1.5 Al 1.5 Si 2 O 14 (CTGAS) single crystal from bulk wave velocities measured by the ultrasonic micro-spectroscopy method. Several plate specimens were cut perpendicular to the X-, Y-, Z-, 35.25°Y-, and 139.74°Y-directions from a CTGAS single crystal ingot grown by Czochralski technique. Following measurements of dielectric constants and density, elastic constants, piezoelectric constants, and their temperature coefficients were determined from longitudinal wave and shear wave velocities measured for the CTGAS specimens at around room temperature. It was demonstrated that the as found constants could provide calculation accuracy within ±0.15% in leaky surface acoustic wave velocity. The determined constants were used for numerical calculation of the cut angle, at which the temperature coefficient of shear wave velocity becomes zero. This angle corresponded to 147.9°Y-cut substrate that had electromechanical coupling factor of k 2 = 3.2%. This parameter is about four times greater than that of AT-cut α-quartz. Introduction: The langasite-type (La 3 Ga 5 SiO 14 : LGS) single crystals are promising materials for pressure sensors operating under high temperature environment as well as highly stable acoustic devices for future communication applications. In particular, the LGS-type crystals are candidate materials alternative to α-quartz from viewpoints of large electromechanical coupling factor, low impedance, and superior temperature stability. In 2000, ordered structure compounds, such as Ca 3 TaGa 3 Si 2 O 14 (CTGS) and Ca 3 NbGa 3 Si 2 O 14 (CNGS), have been developed because the crystals with disordered structure, such as LGS, La 3 Ta 0.5 Ga 5.5 O 14 (LTG) and La 3 Nb 0.5 Ga 5.5 O 14 (LNG) cause high acoustic losses and non-uniform mechanical properties [1]. Fortunately, CTGS and CNGS do not contain costly rare-earth elements unlike LGS, LTG, and LNG. Nevertheless, they still include quite expensive element of Ga. In 2008, Ca 3 TaAl 3 Si 2 O 14 (CTAS) single crystal was successfully developed by substituting 100% of Ga in CTGS with Al and its piezoelectric properties have been evaluated [2, 3]. However, temperature coefficients of the acoustical physical constants (including elastic, piezoelectric, and dielectric constants and density) were not yet reported. These parameters are rather important for designing acoustic devices such as bulk acoustic wave (BAW) resonators and surface acoustic wave (SAW) filters. In addition, physical performance of the mixed crystals formed as a result of partial substitution of Ga 3+ in CTGS with Al 3+ is also not clear. Therefore, examination of acoustic properties of the crystals having intermediate composition of Ca 3 Ta(Ga 1-x Al x) 3 Si 2 O 14 was considered to be important for further understanding of nature of LGS-type materials. Recently, Ca 3 TaGa 1.5 Al 1.5 Si 2 O 14 (CTGAS) bulk single crystals were produced by the Czochralski (CZ) technique [4]. Moreover, in the meantime, a number of single-cryst...