(La, Nd)2/3TiO3 ceramics were prepared through a conventional solid state mixed oxide route. For phase and microstructure analysis, XRD and SEM were used, respectively. Microwave dielectric properties were measured using a network analyzer. XRD patterns revealed the formation of the parent (La, Nd)2/3TiO3 phase along with (La, Nd)4Ti9O24 as a secondary phase. The microstructure consisted of rectangular and needle shaped grains, which decreased in size from 4 μ m to 2 μm with an increase in sintering temperature from 1300 °C to 1350 °C. Decrease in grain size caused an increase in density of the samples from 4.81 g/cm3 to 5.17 g/cm3. Microwave dielectric properties of the samples calcined and sintered in air atmosphere were εr = 40.35, Q × f = 3499 GHz and τ f = 0 ppm/°C, whereas for a sample calcined in nitrogen and sintered in air they were εr = 40.18, Q × f = 4077 GHz and τ f = +4.9 ppm/°C, respectively.