CuInSe2 (CISe) thin films were grown on Mo-coated glass substrates by spray coating technique using nanocrystalline ink. The ink was prepared by dissolving binary CuSe and In2Se3 nanoparticles in iso-butanol. The grown films were subsequently annealed in vacuum and selenium atmosphere, and examined by various characterization techniques. The vacuum-annealed films showed the CuSe binary phase along with the CuInSe2 phase, whereas the selenized films showed a single phase CuInSe2. The elemental analysis of the selenized film exhibited near stoichiometry, and the photoluminescence peak was observed in the region of band-to-band transitions (0.97 eV), which indicated the good structural quality of the selenized films. The developed method opens a new prospect for the finetuning of CISe composition by pre-adjusting the composition of each element in the binary to best fit of CISe in the photovoltaic devices.