Nanocrystalline calcium substituted magnesium titanate was synthesized through an auto‐igniting combustion technique. The phase constitution of the powder was examined using X‐ray diffraction, thermal analyses, and spectroscopic studies. The particle size of ~30 nm was obtained, and that could be sintered to 96% of the theoretic density at 1150°C/2 h. The microstructure of the sintered surface was examined using scanning electron microscopy. The quality factor (Qu × f ) of 65,110 GHz, dielectric constant (εr) of 20.25, and temperature coefficient of resonant frequency (τf) of ~0 ppm/°C suggest that the sintered sample can be used for microwave applications.