With hydrophobic properties and ordered layered structures, mono-n-dodecyloxy-phosphinyl-cerium (terbium) (MDPCT) organic-inorganic hybrid materials were synthesized using cerium nitrate, terbium nitrate and mono-n-dodecyl phosphate (MDP) surfactant with three functions, hydrophobic group and phosphorus precursor, and characterized by XRD, SEM, TEM, FTIR and PLS. The results show that the solvent affects the interlayer spacing, crystallization and luminescent intensity of the prepared MDPCT materials. MDPCT prepared in water exhibits a more ordered layered structure and a higher degree of crystallinity, as well as stronger luminescent intensity than that prepared in ethanol. Based on the excellent solubility in organic solvents, this MDPCT hybrid luminescent material will be a promising candidate for potential biomedical applications in fluorescent imaging and analysis.