The optically controlled tunability of ferroelectric materials is of great interest for use in advanced multifunctional devices. Here, we report the effects of laser with visible (532 nm) and near-infrared (808 and 980 nm) wavelengths on the ferroelectric polarization and electrical properties of [001]-oriented 6Pb(Sc1/2Nb1/2)O-3-61Pb(Mg1/3Nb2/3)O-3-33PbTiO(3) (6PSN-61PMN-33PT) ferroelectric crystal. Our results show that laser irradiation increases the dielectric and piezoelectric properties of this crystal, and their increment is strongly dependent on the wavelength and power of the incident light. Compared with poled crystals, unpoled crystals are more sensitive to light illumination, and a large dielectric increment of approximately 104% (epsilon(r) approximate to 5600) is obtained at ambient temperature using near-infrared 808 nm irradiation. The electrical properties of optically illuminated crystal show good stability, which reverse when the laser is off. These changes in macroscopic behavior are attributed to the laser-induced polarization change in nanoscale size regions. Our results have potential applications in the non-contact optical control of electronic devices.