Thermally conductive green composites are an attractive solution for addressing the escalating heat generation in miniaturized microelectronic devices. They offer simplicity in processing, cost-effectiveness, and the ability to potentially degrade, making them well-suited for overcoming heat-related challenges in next-generation electronics and 5G communication applications. Here, innovative work focuses on developing heat dissipation films by imitating artificial brick–mortar architecture. This approach incorporates cellulose nanocrystals-molybdenum disulfide (CNC-M) nanosheets as bifunctional fillers in polypropylene carbonate (PPC) via straightforward casting technology. This novel composite system leverages CNC-M nanosheets “brick” as oriented bonding and thermal linkers within the PPC “mortar,” significantly enhancing heat transfer across the film, enabling efficient heat propagation and overall thermal conductivity to 3.1 W·m−1·K−1, which is 4450.7 % higher than that of pure PPC. The superior heat dissipation capability enables these composite films to efficiently cool smartphone CPUs, shells, and high-power LED modules. When applying the composite film containing 8 wt% CNC-M to smartphone CPUs and cell phone shells, temperatures decrease by 17.9 °C and 8.3 °C, respectively. Notably, LED modules experience a significant temperature reduction of 22.6 °C. This distinctive “brick–mortar” architecture creates a homogeneous trapezoidal layered architecture that significantly enhances strong hydrogen bonding interactions within a composite film, resulting in exceptional mechanical properties, aging durability, and shape memory. The composite film with 5 wt% CNC-M exhibited impressive increases in tensile strength and Young’s modulus of 152.6 % and 1322.2 %, respectively. Furthermore, the composite film exhibited enhanced UV resistance and based materials. This study advances high-performance thermal conductive materials for electronics thermal management, paving the way for more efficient and sustainable solutions in electronics.
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