With K 2 O as flux, near-stoichiometric In:LiNbO 3 (In:SLN) crystals with different indium contents were grown by the top seed solution growth (TSSG) method. Defect structure characteristics and the replacement principle of extrinsic ions were derived from X-ray powder diffraction, differential thermal analysis (DTA), ultraviolet-visible (UV) absorption and infrared (IR) spectrum measurement. Further analysis indicated that the threshold concentration of In 2 O 3 in near-stoichiometric LiNbO 3 crystals were about 1.1 mol%.