The ferroelectric and piezoelectric properties of Sr2Nb2O7–La2Ti2O7 (SNB-LT) solid solution ceramics have been studied. The La and Ti ions were substituted into the Sr2Nb2O7 (SNB) lattice and their resultant phase of SNB-LT has lattice distortion. The Rietveld refinement parameters from the XRD patterns corroborate a solid solution of Sr2Nb2O7–La2Ti2O7. The addition of La3+ and Ti4+ dampens the SNB intra-structural phase. Raman spectroscopy confirmed the internal lattice relaxation due to the Ti(Nb)O6 octahedron in the lattice. At 2×106 Hz, the dielectric permittivity of SNB-LT-1, SNB-LT-2, and SNB-LT-3 is 17.2, 17.5, and 21.3, respectively, with σac conductivity in the order of 10−5 S/m. With an increase in Ti(Nb)O6 distortion, the piezoelectric coefficient of SNB-LT-1, SNB-LT-2, and SNB-LT-3 increases linearly as 6.3, 8.1, and 9.3 pC/N. The temperature-dependent ferroelectric polarization of SNB-LT-1, SNB-LT-2, and SNB-LT-3 has been tested, and a substantial rise in polarization has been demonstrated up to 120 °C. At 120 °C, the SNBLT solid solution showed a two-fold increase in remnant polarization. Display omitted •Layer perovskites ceramics of Sr2Nb2O7–La2Ti2O7 solid solution prepared with high TC.•Outstanding d33 of ∼0.91 pC/N as well as low σac of 10−5 S/cm at 5 MHz.•Realized good ferroelectricity at 120 °C.