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In this study, Ce2[Zr1−x(Ba1/3Nb2/3)x]3(MoO4)9 (0.02 ≤ x ≤ 0.1, CZ1−xNx) ceramics were sintered at 600 °C and 700 °C using the traditional solid-state method. An analysis conducted through XRD and Rietveld refinement confirmed that all the CZ1−xNx ceramics displayed a single phase with a trigonal structure (space group R-3c). The observed increases in cell volume with increasing x values indicate the successful substitution of (Ba1/3Nb2/3)4+. The high densification of the synthesized phase was validated by the density and SEM results. Additionally, the P-V-L theory demonstrates a strong correlation between the Ce-O bond and εr, as well as τf, and between the Mo-O bond and Q×f. Notably, the CZ0.98N0.02 ceramics demonstrated superior performance at 675 °C, exhibiting εr = 10.41, Q×f = 53,296 GHz, and τf = −23.45 ppm/°C. Finally, leveraging CZ0.98N0.02 ceramics as substrate materials enabled the design of a patch antenna suitable for the 5G communication band, demonstrating its significant potential in this field.