Mg1–3x(CoNiZn)xTa2O6 ceramics (x = 0.00, 0.05, 0.10, 0.20, and 0.25) were synthesized by the solid-phase reaction method. The XRD and Rietveld refinement results suggest that the Mg1–3x(CoNiZn)xTa2O6 ceramics have a pure tri-rutile structure. (Co1/3Ni1/3Zn1/3)2+ can significantly broaden the sintering temperature range of ceramics. The chemical bonding theory reveals that the A-O bond (A = Mg, Co, Ni, or Zn) ionicity and Ta-O bond ionicity are closely related to the porosity corrected relative permittivity (εr-corr.). The increase in A-O bond energy contributes to the greater stability of the AO6 octahedron, resulting in a decrease in |τf|. Additionally, the Raman spectroscopy reveals that there is a negative relationship between the Qf value and the full width at half maximum (FWHM) of the strongest peak of the A1g mode. Correspondingly, Mg0.4(CoNiZn)0.2Ta2O6 ceramic has excellent microwave dielectric properties after sintering at 1450°C for 4 h: εr = 28.9, Qf = 91,900 GHz (at 7.4 GHz), and τf = 44 ppm/°C. Furthermore, Mg0.4(CoNiZn)0.2Ta2O6 ceramic can maintain a stable Qf value (∼ 91,000 GHz) across a broad range of sintering temperatures (150°C), which is a result of the combination of densification and FWHM. This characteristic facilitates adaptation to changes in furnace temperature in large-scale production. The strategy of multiple-element substitution to extend the sintering temperature range is expected to be applied to other ceramic systems.