Ti 4+ -modified MgZrNb 2 O 8 (MgZr 1x Ti x Nb 2 O 8 , x = 0, 0.1, 0.2, 0.3, 0.4) ceramics were synthesized using the traditional solid-state reaction method. Pure MgZr 1x Ti x Nb 2 O 8 was detected without any secondary phase via the X-ray diffraction patterns. According to the sintering behavior and the surface morphology results, the introduction of Ti 4+ reduced the sintering temperature and promoted the grain growth.The correlations between the dielectric properties and the crystal structure were analyzed through the Rietveld refinement and Raman spectroscopy. The slight shifts of the Raman peaks, corresponding to different vibration modes, were induced by the substitution of Ti 4+ for Zr 4+ and related to the improved quality factor. In general, the sample of MgZr 0.9 Ti 0.1 Nb 2 O 8 sintered at 1320°C for 4 h exhibited promising microwave dielectric properties with an ultra-high Q × f value of 130 123 GHz (at 7.308 GHz, 20°C), which is potential for 5G communication applications.