Various methods of synthesis of CuInSe2 remain relevant because it is one of the most effective materials for solar energy. An effective method for the preparation of the CuInSe2 nanodispersed selenium precursor for microwave synthesis is considered. Colloidal selenium solutions were obtained using laser ablation in various liquid media: water, ethanol, triethylene glycol, polyethylene glycol–400 (PEG-400), and a 1% solution of PEG-1500 in PEG-400. The optical properties of the obtained colloidal selenium solutions were studied. Electron microscopy of selenium particles was conducted. Trends of ablation rate change and physicochemical properties of dispersed selenium particles in the variety of liquid media listed above are discussed. The possibility of synthesizing CuInSe2 using the obtained precursor was verified.