In this study, tri-rutile type Mg<sub>0.5</sub>Ti<sub>0.5</sub>TaO<sub>4</sub> ceramics were synthesized, where the structure–property relationship, especially the structural configuration and intrinsic dielectric origin of Mg<sub>0.5</sub>Ti<sub>0.5</sub>TaO<sub>4</sub> ceramics, and the low-firing characteristics were studied. It is found that the tri-rutile structural type is unambiguously identified through the Rietveld refinement analysis, the selected area electron diffraction (SAED), and the high-resolution transmission electron microscopy (HRTEM) along the [110] zone axis. With the increase in sintering temperature, the densification and uniformity of crystal growth play important roles in regulating the microwave dielectric properties of Mg<sub>0.5</sub>Ti<sub>0.5</sub>TaO<sub>4</sub> ceramics. Intrinsically, theoretical dielectric properties calculated by the far-infrared reflective spectra approached the experimental values, indicating the importance of structural features to dielectric properties. Furthermore, a glass additive with high matching relevance with ceramics has been developed to decrease the high sintering temperature of Mg<sub>0.5</sub>Ti<sub>0.5</sub>TaO<sub>4</sub> ceramics, where 2–4 wt% Li<sub>2</sub>O–MgO–ZnO–B<sub>2</sub>O<sub>3</sub>–SiO<sub>2</sub> (LMZBS) glass frit was adopted to reduce the suitable temperature from 1275 to 1050 ℃ without significantly deteriorating the microwave dielectric characteristics. Specifically, Mg<sub>0.5</sub>Ti<sub>0.5</sub>TaO<sub>4</sub> ceramics containing 2 wt% glass addition sintered at 1050 ℃ for 4 h possess excellent microwave dielectric properties: dielectric constant (<i>ε</i><sub>r</sub>) = 44.3, quality factor multiplied by resonant frequency (<i>Q</i>×<i>f</i>) = 23,820 GHz (<i>f</i> = 6.2 GHz), and the temperature coefficient of resonant frequency (<i>τ</i><sub><i>f</i></sub>) = 123.2 ppm/℃.