In order to develop the solid-state laser oscillator based on laser dye compound, the intercalation of rhodamine 6G (R6G) together with cetyltrimethylammonium cations (CTA(+)) into montmorillonite (Mont) interlayer space was investigated. It was found that the solid-material with the light-emitting ability was prepared by cointercalating R6G and CTA(+) molecules into Mont interlayer space at lower molar ratio of R6G to CTA(+) molecules.