Barium strontium zirconate titanate ((Ba 1−x Sr x )(Zr x Ti 1−x )O 3 ; BSZT, x = 0.25 and 0.75) ceramics with a highly crystalline structure were successfully synthesized using the combustion technique, in which urea performed an important role. The effect of calcination (1000-1300 • C) and sintering temperatures (1300-1550 • C) on the phase formation and microstructure of BSZT ceramics were investigated. The pure perovskite phase of BSZT (x = 0.25 and 0.75) powders with a uniform cubic morphology were detected at the calcination temperature of 1300 • C. At the same calcination and sintering temperature, the lattice parameter a of BSZT powder and ceramics with x = 0.75 is higher than x = 0.25. The microstructure of BSZT powders exhibited an almost-spherical morphology and had a porous agglomerated form. The average particle size and the average grain size of all ceramics increased with the increase of calcination and sintering temperatures, but decreased when the content of x increased. The maximum densities of x = 0.25 and 0.75 ceramics were around 5.85 and 5.62 g cm −3 obtained from the samples sintered at 1500 and 1450 • C, respectively.