Langasite (LGS, La3Ga5SiO14) is a promising material in high-temperature piezoelectric devices due to its excellent thermal stability, piezoelectricity, and electrical property. A major challenge in the development of LGS-based devices is to form high-strength bonding of the brittle LGS. Here, we report that the single crystal-single crystal (dual-SC) bonding of LGS is realized through thermal activation under a low compression of 50 kPa for the first time. A record bonding strength of 23.28 MPa is achieved within the dual-SC bonded LGS/LGS structure (with a high bonding ratio exceeding 93%), which is 5 times higher than that of the recent reported LGS/LGS bonding structure (in which a relatively fragile amorphous interface layer is formed between the two LGS samples). The smooth and void-free dual-SC bonding interface of LGS is verified via the cross-sectional transmission electron microscopy (TEM) observations.