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We report a successful fabrication of 0.6Ca0.61Nd0.26TiO3–0.4Nd(Zn0.5Ti0.5)O3 (hereinafter abbreviated as 6CNT–4NCT) microwave ceramics with good sintering activity and desired dielectric properties from EDTA-gel combustion synthesized powders in this paper. The as-synthesized nanopowders have been characterized by X–ray diffraction (XRD), Fourier transformation infrared (FT–IR), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques, respectively. The sintering behavior and dielectric performance have been evaluated on the sintered ceramics. The as-obtained product with amorphous structure could be directly crystallized and produced pure 6CNT–4NCT solid solution phase with orthorhombic perovskite structure at a relatively low temperature of 700 °C, without formation of any intermediate phase. TEM images revealed that homogeneous and well dispersed spherical-shaped nanostructure with an average particle size of 23.8 nm was formed at 800 °C. Well-dense 6CNT–4NCT bulk ceramics with 98.8% relative density were obtained at a relatively low sintering temperature of 1225 °C due to high sintering activity of nanopowders. Moreover, the bulk ceramics exhibited a higher quality factor (Q × f) value than those prepared via the conventional solid-state reaction method. Desired microwave dielectric properties were achieved at 1200 °C: dielectric constant εr = 57.2, Q × f = 59,360 GHz, and temperature coefficient of resonant frequency τf = + 1.95 ppm/°C. This study indicates that the EDTA-gel combustion route is a convenient, low-cost, and interesting route to fabricate high-quality microwave ceramics for practical applications. [ABSTRACT FROM AUTHOR]