Lithium niobate LiNbO 3 crystals were formed at the surface of CuO (1 mol%)-doped 25Li 2 O–25Nb 2 O 5 –50TeO 2 glass (mol%) by heat-assisted (150 ∘ C) continuous-wave Nd:YAG laser irradiations with a wavelength of λ=1064 nm. Nd:YAG laser energies absorbed by Cu 2+ ions (d–d transitions) were converted to the lattice vibrations of surrounding Cu 2+ ions (nonradiative relaxations), giving the increase in the temperature of the laser irradiated local region. The formation of LiNbO 3 crystals was confirmed from micro-Raman scattering spectra. For the line patterned by a laser scanning with a power of 0.59 W and a speed of 6 μm/s, the possibility of a c-axis orientation of LiNbO 3 crystals along the laser scanning direction was proposed. The present study demonstrates that the combination of Cu 2+ and Nd:YAG laser with λ=1064 nm, i.e. transition metal atom heat processing, is effective in inducting LiNbO 3 crystals in TeO 2 -based glasses.