Realizing Remarkable Energy Storage at the Low Earth Orbit Temperature Range in Ternary (2‐ x )SrTiO 3 · x (Bi 0.5 Na 0.5 )TiO 3 ·Bi 4 Ti 3 O 12 Solid Solutions

The high‐performance energy storage ferroelectrics have drawn enormous attention, but one of the challenges for cutting‐edge applications is a limited operating temperature range. Guided by grain boundary structures, composition, and phase field simulation, the remarkable energy‐storage solid solutions were designed using ternary solid solutions 1.6SrTiO 3 ·0.4(Bi 0.5 Na 0.5 )TiO 3 ·Bi 4 Ti 3 O 12 , where giant recoverable energy density U re ∼ 85.0 J/cm 3 , ultrahigh efficiency ƞ ∼ 69.0% and the state‐of‐the‐art frequency stability were realized at Low Earth Orbit temperature range (−180°C–200°C). The emergent dipolar glass states induced by A‐site cationic disorder and size mismatch are the origin of thermal stability and performance retention of 94% at extreme temperatures, which is confirmed by the First Order Reversal Curves method, Arrott plot, and phase field simulation. This work highlights a route to achieve extreme‐temperature energy storage films.