Polycrystalline samples of (Pb0.25Sr0.75)TiO3 (PST75) were prepared by the solid-state reaction method. The effects of firing temperatures and excess PbO on PST75 ceramics were investigated. The PST75 was calcined between 600 and 1000 degrees C for 3 h and the sintering temperature ranged between 1050 and 1250 degrees C for 2 h. The optimized calcination and sintering conditions were identified as 950 and 1250 degrees C, respectively. The lattice parameter c increased, while the lattice parameter a decreased with increased firing temperatures. The average particle size and average grain size increased with increased firing temperatures. After the addition of PbO-excess 0, 1, 3, 5, and 10 wt%-in the PST75 samples, the lattice parameter a decreased. The average particle size and the average grain size increased with the increase of PbO. The porous microstructure slightly decreased with an increasing amount of PbO-up to 3 wt%-then slightly increased with the higher excess PbO. The density was improved by adding 3 wt% of excess PbO. A low dielectric loss was observed from the 3 wt% excess PbO sample.