Flexible, Recyclable, and Highly Conductive Self‐Healing Polymer‐Based Phase Change Films for Thermal Management

Abstract Phase change materials (PCMs) hold significant promise for thermal energy storage and management. However, challenges such as low thermal conductivity, liquid leakage, solid rigidity, and poor recyclability hinder their practical applications. Herein, a facile yet effective strategy for fabricating highly conductive, flexible, and recyclable polymer‐based phase change composites (PCCs) is proposed. The physically crosslinked dual polymer networks endow the PCC film with excellent latent heat (158.6 J g ⁻¹ ), tunable mechanical stress (3.95–8.59 MPa), thermal‐regenerating capability, and recyclability utilization. By utilizing the shear‐induced alignment of graphite nanoplatelets (GNPs), the proposed PCC films demonstrate a remarkable thermal conductivity of 6.24 W m ⁻¹ K ⁻¹ at a GNP loading of 10 wt.%, achieving a thermal conductivity enhancement efficiency of 302%. Moreover, the flexible PCCs‐based energy device demonstrates effective thermal regulation in electronic devices and wearable thermal management. This work provides a cost‐effective avenue for the scalable fabrication of thermally conductive, flexible, and recyclable PCCs toward various thermal management applications.