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Microwave dielectric ceramics (MWDCs) with low dielectric constant and low dielectric loss are desired in contemporary society, where the communication frequency is developing to high frequency (sub-6G). Herein, Nd2(Zr1−xTix)3(MoO4)9 (NZ1−xTxM, x = 0.02–0.10) ceramics were prepared through a solid-phase process. According to X-ray diffraction (XRD) patterns, the ceramics could form a pure crystal structure with the R3¯c (167) space group. The internal parameters affecting the properties of the ceramics were calculated and analyzed by employing Clausius–Mossotti relationship, Shannon’s rule, and Phillips–van Vechten–Levine (P–V–L) theory. Furthermore, theoretical dielectric loss of the ceramics was measured and analyzed by a Fourier transform infrared (IR) radiation spectrometer. Notably, when x = 0.08 and sintered at 700 ℃, optimal microwave dielectric properties of the ceramics were obtained, including a dielectric constant (εr) = 10.94, Q·f = 82,525 GHz (at 9.62 GHz), and near-zero resonant frequency temperature coefficient (τf) = −12.99 ppm/℃. This study not only obtained an MWDC with excellent properties but also deeply analyzed the effects of Ti4+ on the microwave dielectric properties and chemical bond characteristics of Nd2Zr3(MoO4)9 (NZM), which laid a solid foundation for the development of rare-earth molybdate MWDC system.