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Abstract Defect chemistry that results in the thermal processing of dielectric and piezoelectric films, crystals and ceramics ultimately controls the properties and long‐term performance of materials and devices. This paper reviews several thermochemical defect reactions using important perovskite base composition dielectrics including Pb(Zr,Ti)O₃, (Na,K)NbO₃, (Bi_0.5Na_0.5)TiO₃‒BaTiO₃, and Ca(Hf,Ti,Mn)O₃. Within this group of perovskite‐based functional materials, we note ways the point defects can be formed to create non‐stoichiometric compositions changing the overall cation‐to‐anion ratios during the synthesis process. These reactions can be developed with the loss of volatile species such as metal and oxygen ions. The relative concentrations of these can impact the over conductions in terms of the mixed contributions of ionic conductivity from the oxygen vacancies and the electronic conductivity, along with microstructure and properties in some cases.