The domain configuration was reengineered with a modified poling procedure for the [011]-poled single-domain PMN-0.35PT crystals located at the morphotropic phase boundary. As a consequence, the dielectric constant epsilon(r) at room temperature was significantly enhanced by more than 10 times to about 18 000, extremely higher than the reported (1 - x)Pb(Mg1/3Nb2/3)O-3-xPbTiO(3) ferroelectric crystals. Besides, the decreasing rate of the dielectric constant (d epsilon(r)/dT) was about 300/K with a temperature coefficient () of 1.7%/K, comparable to the BST materials for dielectric bolometer applications. The ferroelectric phase transition behavior was investigated to establish the poling procedure and a thermal hysteresis of about 25 degrees C was indicated across the room temperature for the orthorhombic-tetragonal phase transition, which contributed to the revolution of the domain pattern.