A series of Eu3+/Tb3+/Tm3+ single/co-doped NaLa(MoO4)2 (NLM) phosphors have been synthesized by microemulsion-hydrothermal method. Phosphor crystal structure, morphology and luminescent properties were tested and studied by X-ray diffraction (XRD), scanning electron microscopy (SEM) and fluorescence spectroscopy. The results show that the prepared samples are all tetragonal single crystals. By way of substitution, the sites of La3+ are replaced by Eu3+, Tb3+and Tm3+. Morphology of the samples are tetragonal sheet structure and the size of particles is 1~1.5 μm. When the doping concentration of Eu3+ is 9%, NLM∶9%Eu3+ phosphor emission peak is the strongest at 616 nm, the critical transfer distance (Rc) between Eu3+ in the NLM matrix is about 15.20  at this time. At the emission spectrum of NLM∶9%Eu3+, the peak at 591 nm is the magnetic dipole transition of 5D0 to 7F1 of Eu3+. The peak at 616 nm is the electric dipole transition of 5D0 to 7F2 of Eu3+. Electric dipole transition emission intensity is about 10 times of the strength of the magnetic dipole transition. This indicates that Eu3+ is located at noninversion symmetry site. By Fixing Eu3+ (Tb3+) concentration and varying the concentration of Tb3+ (Eu3+), the energy transfer mechanism between Eu3+ and Tb3+ was studied. By adjusting the Eu3+, Tb3+and Tm3+ doping concentrations, tunable luminescence of visible light region is implemented under the single matrix. The luminescence of NLM∶x%Eu3+, y%Tb3+, z%Tm3+ phosphors are translated from blue (0.205, 0.135) to pseudo-white (0.305, 0.266) under 360 nm irradiation.