The changes in the degree of structural imperfection of lithium niobate (LiNbO 3 ) single crystals with an increase in the Li content and doping with zinc (to 1 wt %) have been investigated by the nonlinear optics methods and Raman spectroscopy. The conversion of broadband IR radiation in LiNbO 3 crystals under noncritical (90°) phase matching condition with vector interactions implemented is investigated. It is shown that the conversion efficiency, spectral width, and the position of maximum in the converted radiation spectrum depend on the ratio R = Li/Nb in LiNbO 3 crystal and the impurity concentration.