0.695Pb(Mg1/3Nb2/3)O-3-0.305PbTiO(3) (PMN-0.305PT) single crystals were grown by a modified Bridgman method. X-ray powder diffraction (XRPD) and X-ray single crystal diffraction (XRSCD) measurements showed that the crystal structure of PMN-0.305PT can be identified as distorted rhombohedral structure or triclinic structure, with both close to pseudo-cubic structure. Polarization exerts significant influences on electrical properties, domain configuration, and infrared spectra of the PMN-0.305PT crystal plates with different orientations. An additional dielectric peak or dielectric shoulder is induced at lower temperature in the dielectric response behavior, in which the shape and temperature of the dielectric anomaly exhibit great dependency on the crystal orientation. The PMN-0.305PT single crystals exhibit complex domain configuration with statistical 4 mm symmetry after poling. The stretching normal vibration of [Mg1/3Nb2/3]/TiO3 group is observed in the fourier transform infrared spectroscopy (FT-IR) spectra with infrared-absorption band occurring around 609 cm(-1). The PMN-0.305PT single crystals exhibit excellent pyroelectric property, which will lead to promising advance in pyroelectric applications.