(1–x)CaTiO3–xNdAlO3 (CTNA) microwave dielectric ceramics have a high Q value and a low temperature coefficient of resonant frequency ( τf ). CTNA ceramic powder was synthesized using a polymeric precursor derived from a mixed-metal ethylenediaminetetraacetic acid (EDTA) / ethylene glycol solution. The precursors and derived oxide powders were characterized by thermogravimetric analysis and X-ray diffraction. When x = 0.3, CTNA was synthesized at 900°C for 3 h in air. Compared with that prepared by the solid-state reaction method in literatures, the CTNA ( x = 0.3 ) ceramics with better microwave properties could be obtained at lower calcination and sintering temperatures by EDTA chelating method.