Two-dimensional (2D) perovskite-like slabs are a class of materials that are structurally identical but have one direction of reduced dimensionality, giving the material a layered or sheet-like structure. Such materials have outstanding dielectric properties in ceramics. Such ceramic compositions of (SrxCa1−x)3Ti2O7 (0.2 ≤ x ≥ 0.8) were synthesized using the solid-state technique. The phase, microstructural and microwave dielectric properties of dense sintered (SrxCa1−x)3Ti2O7 ceramics (0.2 ≤ x ≥ 0.8) were analyzed by X-ray diffraction (XRD), Scanning electron microscopy (SEM), Fourier transformed infrared spectroscopy (FT-IR) and impedance analysis. All the samples have a Tetragonal phase structure with a space group of I4/mmm formation and the crystalline size, dislocation density and lattice strain changes with respect to Sr2+ doping were observed in the XRD analysis. The Fourier Transform Infrared Spectra (FT-IR) confirmed the bonding characteristics of CaCO3, TiO2 with SrCO3. The dielectric constant (εr) increased from 6.02 to 42.5 while minimum tangent loss (tan δ) observed was 0.0015.