The (1– x)Ca 0.61La 0.26TiO 3- xNd(Mg 0.5Ti 0.5)O 3 [(1– x)CLT- xNMT, x = 0.35~0.60] ceramics were prepared via microwave sintering. The effects of sintering temperature and composition on the phase formation, microstructure, and microwave dielectric properties were investigated. The results show that the microwave sintering process requires a lower sintering temperature and shorter sintering time of (1– x)CLT- xNMT ceramics than conventional heating methods. All of the (1– x)CLT- xNMT ceramics possess a single perovskite structure. With the increase of x, the dielectric constant ( ε) shows a downward trend; the quality factor ( Qf) drops first and then rises significantly; the resonance frequency temperature coefficient ( τ f ) keeps decreasing. With excellent microwave dielectric properties ( ε = 51.3, Qf = 13,852 GHz, τ f = −1.9 × 10 −6/°C), the 0.65CLT-0.35NMT ceramic can be applied to the field of mobile communications.