Rare earth ions doped luminescence nanomaterials have broad applications ranging from television tubes to biological imaging. A series of Yb3+ /Er3+ /Eu3+ ions doped NaGdF4 dual-mode (up- and down-conversion) luminescence phosphors have been prepared by L-arginine assisted-hydrothermal method. The results show that the synthesized samples are all pure beta-NaGdF4 with one dimensional micron structure. Changing the excitation wavelengths and Eu3+ ion concentrations, multiple (yellowish green, yellow, orange) emissions are obtained. Moreover, the energy transfer, luminescence mechanism and paramagnetic properties of the samples have been discussed in this paper.