Two kinds of scheelite-structure microwave dielectric ceramics with I41/a space group were prepared by the conventional solid-phase reaction method. The effects of different sintering temperatures on the crystal structure, lattice vibration and microwave dielectric properties of NaSrLn(MoO4)3 (Ln = Nd, Sm) ceramics were investigated. XRD and Rietveld refinement results show that NaSrLn(MoO4)3 (Ln = Nd, Sm) ceramics belong to tetragonal scheelite structure with I41/a space group. The lattice vibration mode was analyzed by Raman spectroscopy, and the correlation between the dielectric performances and structure was established. The NaSrLn(MoO4)3 (Ln = Nd, Sm) ceramics have high density (>97%) and excellent microwave dielectric properties of εr = 10.47, Qf = 38951 GHz, τf = −48.43 ppm/°C for NaSrNd(MoO4)3 sintered at 775 °C and εr = 9.55, Qf = 41081 GHz, τf = −44.92 ppm/°C for NaSrSm(MoO4)3 sintered at 800 °C. In addition, NaSrLn(MoO4)3 (Ln = Nd, Sm) ceramics have excellent chemical compatibility with Ag electrodes, which means that the ceramic could be used in LTCC microwave devices.
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