This study presents the microwave dielectric properties calculation of (1-x)Ba 3.75 Nd 9.5 Cr 0.25 Nb 0.25 Ti 17.5 O 54 -xNdAlO 3 ceramics where x denotes the volume molar fraction. From X-ray diffraction results, the solid solution limit is calculated to be about 0.76, where it forms a single BaNd 2 Ti 4 O 12 phase in Region I (0 ≤ x ≤ 0.76), and both BaNd 2 Ti 4 O 12 and NdAlO 3 coexist in Region II (0.76 < x < 1). The solid solution limit is confirmed by independently calculating it from the dielectric constant data. There is less than 4 % deviation between the measured dielectric constant (ε r ) and the one calculated from the Maxwell-Wagner formula. The total quality factor (Q) remains almost constant in Region I and increases rapidly with the volume molar fraction of NdAlO 3 in Region II. The measured Q×f, where f is the resonant frequency, is also consistent with the calculated value in both regions. The temperature coefficient at the resonant frequency is -1.4 ppm/ o C, which agrees well with the calculated value of 0 ppm/ o C. In addition, we observed a close correlation between the bulk density and the phase evolution.