The development of fluorescent materials with low energy consumption, low cost and desirable optical properties is needed for the perspective of practical application. Here, functional NaLa(MoO4)(2)@CdTe core-shell microspheres with high fluorescence were prepared by layer-by-layer self-assembly technique. Through the consecutive electrostatic adsorption of charged cetyltrimethyl ammonium bromide and CdTe quantum dots (QDs), the uniform and regular multilayer shell of CdTe QDs was synthesized. The NaLa(MoO4)(2)@CdTe microspheres exhibited improved photoluminescence intensity and stability of red emission, compared with that of the CdTe QDs powder, and the fluorescence enhancement mechanism were investigated. The CdTe QDs multilayer shell is expected to supersede the Eu3+ ion for producing a novel red phosphor.