Ultra‐Dense Bottlebrush Dynamic Phase Change Polymer Networks with Ultra‐High Latent Heat and Adaptive Electrically Conductive for Intelligent Thermal Storage and Device

Abstract Conventional thermal energy storage systems employing phase change materials (PCMs) intrinsically lack capabilities for real‐time state monitoring, leading to unpredictable energy storage status and performance deficiencies in meeting the precision thermal requirements of the Internet of Everything. Here, the adaptive electrically conductive and highly energy‐dense PCMs using ultra‐dense bottlebrush networks with metal‐coordinated crosslinking are reported. This topological design achieves a breakthrough latent heat of over 200 J g −1 based on maximizing entropy variation through boosted phase‐change unit content and minimizing entanglements. By coupling between dissociation and migration of metal ions as well as phase transition‐induced segmental relaxation, adaptive electrical conductivity can be achieved, enabling a transition of PCMs from insulating to conductive along with enthalpy change. The unique PCMs enable real‐time thermal energy storage monitoring and can be processed into thermally regulated photolithographic circuits. These dual breakthroughs in energy density and intrinsic responsiveness render this transformative material suitable for thermal engineering and device regulation.