This study investigates the effects of lithium (Li) and potassium (K) additions on the microstructure, densification, and microwave dielectric properties of (A 1+ 0.5 Nd 3+ 0.5 )TiO 3 to CaTiO 3 resulting new ceramic complex with new microwave dielectric properties. The (1-x)CaTiO 3 -x(Li₀. 5 Nd₀. 5 )TiO 3 ceramics were synthesized with x values of 0.08, 0.1, 0.2, 0.5, and 0.9 mol.%, and (1-x)CaTiO 3 -x(K₀. 5 Nd₀. 5 )TiO 3 ceramics with x values of 0.02, 0.05, 0.08, 0.10, 0.20, 0.50, 0.90, and 1.0 mol.% via the solid-state method. The results reveal that both the type and concentration of the alkali significantly influence the dielectric properties. The 92CTLNT ceramic (x = 0.08), sintered at 1200°C, exhibited excellent dielectric properties with a dielectric constant (ε r ) of 27, Qxf value of 1.38 × 10 4 at 5 GHz, and a low dielectric loss of 0.37 × 10⁻ 3 . Meanwhile, the 98CTKNT ceramic (x = 0.02), sintered at 1300°C, showed superior performance with ε r of 40, a Qxf value of 3.33 × 10 4 at 4 GHz, and a low dielectric loss of 0.13 × 10⁻ 3 .The exceptional microwave dielectric properties of these ceramics present significant potential for advanced applications in microwave and communications technologies.