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Phase change materials (PCMs) are regarded as promising candidates for realizing zero‐energy thermal management of electronic devices owing to their high thermal storage capacity and stable working temperature. However, PCM‐based thermal management always suffers from the long‐standing challenges of low thermal conductivity and liquid leakage of PCMs. Herein, a dual‐encapsulation strategy to fabricate highly conductive and liquid‐free phase change composites (PCCs) for thermal management by constructing a polyurethane/graphite nanoplatelets hybrid networks is reported. The PCM of polyethylene glycol (PEG) is first infiltrated into the cross‐linked network of polyurethane (PU) to synthesize hybridized semi‐interpenetrated composites (PEG@PU), and then incorporated with reticulated graphite nanoplatelets (RGNPs) via pressure‐induced assembly to fabricate highly conductive PCCs (PEG@PU‐RGNPs). The hybrid networks enable the PCCs to show excellent mechanical strength, liquid‐free phase change, and stable thermal property. Notably, the dual‐encapsulated PCCs exhibit high thermal and electrical conductivities up to 27.0 W m−1 K−1 and 51.0 S cm−1, superior to the state‐of‐the‐art PEG‐based PCCs. Furthermore, the PCC‐based energy device is demonstrated for efficient battery thermal management toward versatile demands of active preheating at a cold environment and passive cooling at a hot ambient. Overall, this work provides a promising route for fabricating highly conductive and liquid‐free PCCs toward thermal management.

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Solar thermal energy conversion and storage within phase change materials (PCMs) can overcome solar radiation intermittency to enable continuous operation of many heating-related processes. However, the energy-harvesting performance of current storage systems is always limited by low efficiencies in either solar thermal energy conversion or thermal transport within PCMs. Although PCM-based nanocomposites can address one or both of these issues, achieving high-performance composites with simultaneously enhanced photothermal performance and thermal transport capacity remains challenging. Here, we demonstrate that dual-functional aligned and interconnected graphite nanoplatelet networks (AIGNNs) yield the synergistic enhancement of interfacial photothermal conversion and thermal transport within PCMs to accelerate the solar thermal energy harvesting and storage. The AIGNNs include the naked part as the three-dimensional optical absorber and the incorporated part as thermally conductive pathways within PCMs. First, a phase change composite composed of the AIGNNs and the solid–solid PCM of polyhydric alcohol is synthesized using a facile three-step method, and shows 400% thermal conductivity enhancement for per 1 wt % graphite loading compared to pristine PCMs. After the elaborate surface treatment, a small part of the graphite networks is in situ exposed as the 3D optical absorber to boost the surface full-spectrum sunlight absorptivity up to 95%. This dual function design takes full advantage of the integrated AIGNNs in terms of both photothermal conversion and thermal transport capacities, superior to the traditional coating-enhanced photothermal conversion. This work offers a promising route to accelerating solar thermal energy harvesting and storage within PCMs.

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