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$$\upalpha $$ - $$\hbox {LiIO}_{3}$$ is an excellent optical material exhibiting strong nonlinear optical, piezoelectric and elasto-optic properties. However, its practical applications are limited by the insufficient reproducibility of the mentioned properties caused by the strong influence of the growth conditions, and, in particular, pH of the solution from which $$\upalpha $$ - $$\hbox {LiIO}_{3}$$ crystal is grown. Herein, we investigate to grow bulk size good quality crystals of $$\upalpha $$ - $$\hbox {LiIO}_{3}$$ based on the observed problems during its crystallization process. A systematic investigation was carried out to find the effect of pH on solubility, crystal growth, structural, surface and laser damage properties of $$\upalpha $$ - $$\hbox {LiIO}_{3}$$ single crystals. The structure and phase of $$\hbox {LiIO}_{3}$$ were confirmed by powder X-ray diffractometer analysis. The functional groups of the compound were identified using Fourier transform infrared spectroscopy. Surface defects of the grown crystals were studied by etch patterns. The crystal grown at pH 10 showed 10% optical transmission enhancement in comparison to the crystals grown at pH 2. The indirect optical bandgap of the crystal was reinvestigated using ultraviolet-Visible-near-infrared transmittance spectrum. The laser damage threshold studies of the crystals grown at pH 10 reveal the higher optical radiation stability against 532 nm laser. The second-order nonlinear optical behaviour of $$\upalpha $$ - $$\hbox {LiIO}_{3}$$ crystals grown at different pH conditions have been investigated by using Kurtz and Perry powder technique with Nd:YAG laser pulses at the wavelength of 1064 nm. [ABSTRACT FROM AUTHOR]