The microstructure and microwave dielectric characteristics of (Ba 0.98 Sr 0.02 ) 3.75 Nd 9.5 Ti 18-x (Zn 1/3 Nb 2/ 3 ) x O 54 ceramics solid solutions (0 B x B 2.5) were investigated in this study. X-ray diffraction indicated that only BaNd 2 Ti 4 O 12 existed in the sintered samples when x value was lower than 2.0, but subsequently a new phase generated with increasing of x value. The dielectric constant (e r ) of the samples increased slightly from 83.4 to 85.2 before falling down and quality factor value (Q 9 f) declined radically from 10,873 to 1321 GHz at optimum sintering temperature of 1450°C, as x value increased from 0.0 to 2.5. And the temperature coefficient of resonant frequency (s f ) could be adjusted to a minimum value and then rebounded because of the second phase NdNbTiO 6 which also sharply deteriorated the quality factor of the samples. At last, the excellent microwave dielectric properties of the samples with values of e r = 85.2, Q 9 f = 5989 GHz, s f = ?14.9 ppm/°C were obtained as x was 1.0 sintered at 1450°C for 3 h in air.