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Regarding advanced 5G mobile communication, microwave dielectric ceramics are considered as the most potential materials to develop new-generation base station resonators. Herein, ZnNb 2 O 6 ceramics with ε r of approximately 24 have been prepared using the solid-state reaction method, with tailored extra ZnO of x mol% (x = 1, 2 and 3). We have for the first time applied the P-V-L chemical bond theory to investigate ZnNb 2 O 6 ceramics with ZnO doping, by exploring the relationship of dielectric properties and chemical bond characteristics. Particularly, the Raman spectra demonstrates that the full width at half maximum of υ 1 (A g) vibration mode can exhibit significant correlation with the quality factor (Q × f). To further support the experimental study, we have also conducted the first-principle calculation of electron density difference via CASTEP package, which further confirms the change of temperature coefficient of resonance frequency (τ f). Our newly designed ZnNb 2 O 6 ceramics doped with 1 mol% ZnO exhibit excellent dielectric properties, i.e., ε r = 23.74, Q × f = 102,824 GHz and τ f = −55.38 ppm/°C, which demonstrates great potential to construct miniaturized 5G base station with advanced ceramic dielectrics. [ABSTRACT FROM AUTHOR]