Using various amounts of TiO2, the 0.65CaTiO(3)-0.35Sm(0.9)Nd(0.1)AlO(3) ceramics were prepared via the conventional solid-state reaction method. The relationships between the crystalline structure and microstructure, as well as the microwave dielectric properties, were investigated. The sintered ceramics formed a solid solution, and short-range ordering at B-site ions was detected by Raman spectroscopy. A slight amount of Al-rich secondary phase was observed along the grain boundary, which increased with the TiO2 content. The additional TiO2 promoted the densification of ceramics and positively affected the dielectric constant, epsilon(r) and the temperature coefficient of resonant frequency, tau(f).Nevertheless, the excess Al-rich secondary phase destroyed the short-range ordering of the B-site ions and deteriorated the Q x f value. Considering all three parameters of the microwave dielectric properties, the 0.25 wt% TiO2-modified 0.65CaTiO(3)-0.35Sm(0.9)Nd(0.1)AlO(3) ceramic exhibited the best performance of epsilon(r) = 40.43, Q x f = 51531 GHz and tau(f) = -3.7 ppm/degrees C sintered at 1445 degrees C for 3 h. (C) 2013 Elsevier Ltd. All rights reserved.