Sulfosalicylic acid (SSA) was used as an intercalation agent and an excellent antenna to synthesize layered rare-earth hydroxide (LRH) materials and directly obtain SSA-modified terbium-doped ytterbium hydroxide nanosheets by mechanical exfoliation. The crystal structure and morphologies of the LRHs and nanosheets were determined by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The particle size and zeta potential of the prepared nanosheets were also analyzed. The as-prepared nanosheets exhibited excellent luminescent properties. The positively charged nanosheets were electrophoretically deposited on a conductive glass to form a thin film. The luminescence of this thin film can be quenched by chromate (CrO 4 2–) and bilirubin (BR), which shows good sensing properties. The quenching mechanism of the sensing film by CrO 4 2– and BR was discussed based on the spectra and structure of the film.