We explore piezooptic and photoelastic properties of Ca3Ga2Ge4O14 (CGG) crystals. A Mach–Zehnder interferometry technique is utilized to determine a complete set of the piezooptic tensor constants πim, with particular attention to the measurement accuracy, reliability, and uncertainty resolution in the piezooptic measurements. For these reasons, independent piezooptic constants or their combinations were determined by performing interferometric measurements for different geometries of piezooptic coupling using samples of both principal (direct) and non-principal (X/45°) crystallographic cuts. Basing on the results of piezooptic measurements, a complete set of photoelastic tensor constants pim and the acousto-optic performance (figure of merit M2) of CGG crystals were evaluated. The obtained piezooptic, photoelastic, and acousto-optic characteristics of CGG crystals are compared with those of other crystals of the langasite group, langasite and CTGS (Ca3TaGa3Si2O14). A comparative analysis reveals a correlation between the values of the piezooptic or photoelastic constants and the lattice parameters for this group of crystals. High optical quality and optical transparency in the UV region of the spectrum up to 260 nm together with extremely high mechanical resistance to uniaxial compression (≤2000 kg/cm2) opens up the possibility for specific application of CGG crystal as an optical material for piezooptic sensors of high uniaxial compression. The presented piezooptic interference technique along with methodological and metrological approaches paves the way for accurate and unambiguous characterization of photoelastic crystal materials of trigonal symmetry.