Lead Magnesium Niobate Titanate 0.74 Pb(Mg1/3Nb2/3)O3-0.26PbTiO3 (0.74PMN-0.26 PT) single crystal doped with 1 mol% Nd3+ was grown by a modified Bridgman approach. Powder X-ray diffraction exhibited perovskite structure containing rhombohedral phase. The dielectric constants of various orientations with temperature were determined. We observed that the polarization process increases the crystal optical performances. The transmittance is significantly increased after poled along [011] direction. Optical properties changes were interpreted by electric domain structure. Energy band gaps were obtained by Tauc equation. Nd3+ has a strong emission transition band near 1062 nm; the long radiation lifetime of 148 μs indicates a low quenching effect. For the Nd-doped PMN-PT single crystals, their optical and electrical performances have been explored to extend the applications in medical, military and practical industrial production.