Large and crack-free LiInSe2 single crystals were obtained by the vertical gradient freezing method with adding a temperature oscillation technology in a two-zone furnace. X-ray diffraction data showed that the pure LiInSe2 compound was synthesized. The grown crystals had different color depending on melt composition. The atomic ratios of elements of LiInSe2 crystals were obtained by an Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES), and the structural formula were calculated according to the relative contents of elements. The average absorption coefficients were estimated by using average reflection indices. The absorption coefficients of the thermal annealing samples are similar to 0.6 cm(-1) at similar to 2-3 mu m. The transparent range of our LiInSe2 crystals is from 0.6 mu m to 13.5 mu m. (C) 2014 Elsevier B.V. All rights reserved.