The sol-gel method was used to synthesize two different Ba0.75Sr0.25Ti0.95Zr0.05O3 powders: one of high purity and the other of low purity. These two sol-gel-synthesized powders show two distinct particle sizes and surface areas. The slip casting method was applied to these two sol-gel powders followed by a pressureless sintering, which shows large differences in sintered density and grain size for the pressureless sintered disks. Neutron powder diffraction shows a transition to the nonpolar cubic Pm-3m space group at higher temperatures for both materials. Pair distribution function analysis was used to examine the local displacements of the Ti4+ and Zr4+ cations. The dielectric constant, loss tangent, and bias were measured on these two materials.