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High-quality-factor and low temperature coefficient of the resonant frequency Ca0.66Ti0.34La0.3Al0.3O3 ceramics had been prepared by the conventional solid-state reaction method,and their microwave dielectric properties had been investigated.LnO and LnAlO3 (Ln=La,Sm,Nd) were selected as additive to adjust the microstructure and dielectric of Ca0.66Ti0.34La0.3Al0.3O3 ceramics.Excess LnO and LnAlO3 in the range of 0–3.5 wt% was added.It was found that these additives had great influence on the microstructure and microwave dielectric properties of Ca0.66Ti0.34La0.3Al0.3O3 ceramics.