The doped 0.25Pb(Mg1/3Nb2/3)O3–0.40PbTiO3–0.35PbZrO3 (PMN–PZT) ceramics with pure perovskite phase were prepared by one-step oxide-mixed method and conventional columbite method. The phase structure and electrical properties were systematically investigated. Crystallites of the ceramic fabricated by the oxide-mixed method are partially oriented with the c-axis, while samples prepared from columbite method are randomly oriented. This crystalline orientation enabled better electric properties, especially a higher piezoelectric coefficient d33 of 760 pC/N and electromechanical coupling factor kp of 69%. Materials fabricated from the oxide-mixed method are attractive for high-performance piezoelectric actuator and this simple method may have a great prospect in industrial production.