Temperature-dependent acoustic loss Q−1 is studied in partially disordered langasite (LGS, La3Ga5SiO14) and ordered catangasite (CTGS, Ca3TaGa3Si2O14) crystals and compared with previously reported CTGS and langatate (LGT, La3Ga5.5Ta0.5O14) data. Two independent techniques, a contactless tone-burst excitation technique and contacting resonant piezoelectric spectroscopy, are used in this study. Contributions to the measured Q−1(T) are determined through fitting to physics-based functions, and the extracted fit parameters, including the activation energies of the processes, are discussed. It is shown that losses in LGS and CTGS are caused by a superposition of several mechanisms, including intrinsic phonon–phonon loss, point-defect relaxations, and conductivity-related relaxations.