Optical hybrid materials based on inorganic hosts and organic sensitizer guests hold promise for a virtually unlimited number of applications.In particular,the interaction and the combination of the properties of a defined inorganic matrix and a specific sensitizer could lead to synergistic effects in luminescence enhancing and tuning.The current article focuses on the intercalation assembly of optical hybrid materials based on the layered terbium hydroxide(LTbH) hosts and organic divalent carboxylic sensitizer anion guests by a hydrothermal process.The studies on the interactions between hosts and guests indicate that the type and arrangement of organic guests in the layer spacing of the LTbH hosts can make a difference in the luminescence of the hybrid inorganic-organic materials. Optical hybrid materials based on inorganic hosts and organic sensitizer guests hold promise for a virtually unlimited number of applications. In particular, the interaction and the combination of the properties of a defined inorganic matrix and a specific sensitizer could lead to synergistic effects in luminescence enhancing and tuning. The current article focuses on the intercalation assembly of optical hybrid materials based on the layered terbium hydroxide (LTbH) hosts and organic divalent carboxylic sensitizer anion guests by a hydrothermal process. The studies on the interactions between hosts and guests indicate that the type and arrangement of organic guests in the layer spacing of the LTbH hosts can make a difference in the luminescence of the hybrid inorganic-organic materials.