Complex perovskites of the formula (Ba 1=3 Ln 2=3 )(Zn 1=3 Ti 2=3 )O 3 (Ln ¼ La, Pr, and Nd) and (Ba ð1þxÞ=3 La ð2ÀxÞ=3 )(Zn 1=3 Ti ð2ÀxÞ=3 Nb x=3 )O 3 (x ¼ 0:5; 0:75; 1:0; 1:25) have been synthesized by solid state reactions and are found to crystallize in the cubic structure (space group Pm 3 3m) from Rietveld refinement of powder X-ray data. The lattice parameter and the grain size increases with Nb substitution. Among the above oxides, (Ba 1=3 La 2=3 )(Zn 1=3 Ti 2=3 )O 3 shows the best dielectric properties with quality factor (Q) of 3139 at 6.67 GHz and a temperature coefficient of resonant frequency ( f ) of À10:8 ppm/ C. Further, the temperature coefficient of resonant frequency ( f ) shows a large and systematic variation (with a continued decrease and a change of sign from positive to negative) with increase in Nb content.