Rare earth luminescent materials have broad application prospects in the fields of white light LED lighting, flat panel display, biological imaging and so on. Here, we developed a novel silicate clay minerals-based montmorillonite nanosheet(Mt)/YF3:Eu3+ nanocomposites with strong luminescence performance. Mt carrier plays a three role: (1) reducing the size and improving dispersion of YF3: Eu3+ nanoparticles by surface effect; (2) narrowing down the band gap and increasing Urbach tail energy by interface effect; (3) reducing the shielding of the hole-electron Coulomb interactions while improving the exciton binding energy of YF3:Eu3+, thus improving the radiative recombination by dielectric effect. Therefore, orthogonal phase YF3: Eu3+ nanoparticles (diameter 20∼140 nm) binding to the surface of Mt via chemical bond interactions. The combination of Mt and YF3:Eu3+ not only enhanced luminescent intensity (about 2 times) but also improved the quantum yield (0.14% to 0.4%) and fluorescence lifetime (0.338 ns to 0.405 ns) of YF3:Eu3+ nanoparticles at 595 nm. In addition, the combination of Mt and YF3:Eu3+ give luminescent properties to Mt thereby improving the utilization rate of Mt and YF3: Eu3+ nanoparticles. It was found that the research supplies an insight on the development of new type luminescent materials, and hopefully it could promote them application in many fields.