Ferroelectric crystal Pb(Lu1/2Nb1/2)O3–0.2PbTiO3 (PLN–0.2PT) was successfully obtained by a top-seed solution growth technique. At room temperature the symmetry was orthorhomic according to X-ray diffraction (XRD). The super-lattice reflections were identified by XRD and transmission electron microscope (TEM). The micro-domain structure was detected by TEM. The temperature dependence of the dielectric constant (ϵ′) shows a typical relaxor behavior. The temperature dependence of coercive electric field and remnant polarizations were investigated, which also shows the relaxor feature.