New high-ɛ and high-Q microwave dielectric ceramics (1−x)Ca 0.61 Nd 0.26 TiO 3 −xNd(Zn 0.5 Ti 0.5 )O 3 (x=0.00–0.40, referred to as (1−x)CNT−xNZT) were prepared by conventional solid-state preparation route. Single orthorhombic perovskite phase was formed when x was not beyond 0.15. And a secondary phase Zn 2 TiO 4 appeared for x=0.20, while ZnO was the secondary phase for the ceramics with x above 0.20. The dielectric constant and temperature coefficient of resonant frequency decreased steadily with increasing x-value. High Qf-value of above 10,000GHz was achieved as x varied from 0.00 to 0.20. However, Qf-value decreased rapidly when x was beyond 0.20. Some (1−x)CNT−xNZT ceramics with high ɛ and high Qf value were obtained: ɛ=78.8, Qf=19,200GHz, τ f =+135ppm/°C for x=0.15; ɛ=71.8, Qf=17,300GHz, τ f =+94ppm/°C for x=0.20.