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With the rapid development of portable electronic devices, there is an urgent need for the multifunctional composites like excellent electromagnetic interference (EMI) shielding performance, mechanical property, and thermal management capabilities. Here, due to the low thermal conductivity of phase change materials (PCMs), a sandwich structure carbon nanotube/phase change microcapsule/carbon nanotube (CNT/PMC/CNT (CPC)) film was prepared by vacuum‐assisted filtration (VAF) method. CNT, PMC, and cellulose nanocrystal (CNC) were used as functional fillers. The addition of CNCs was used to improve the mechanical performance of CPC film. Compared with PMC‐CNC (PC) film, CPC film with sandwich structure prevented leakage phenomenon efficiently. Subsequently, the use of ultrasonic‐assisted forced infiltration (UAFI) successfully infiltrated polydimethylsiloxane (PDMS) matrix in the filler skeleton to obtain CNT/PMC/CNT/PDMS (CPCP) composites. When filler mass ratio (CNT: CNC and PMC: CNC) reached 10:1, the thermal conductivity of CPCP composites was 2.32 W/(m·K) and total EMI shielding effectiveness (EMI SET) of it with 0.38 mm thickness reached 37.46 dB at 12.4 GHz. Besides, these sandwich composites exhibited the good mechanical properties and heat storage capacity. And we systematically observed the impact of different addition amounts of PC homogeneous dispersing solution on phase change ability of CPCP10:1 composites. In summary, CPCP phase change composites with sandwich structure shows potential application prospect in thermal management materials with EMI shielding of electronic devices. Highlight: The sandwich structure CPCP composites prepared by the combination of VAF and UAFI method, showing superior thermal conductivity and phase change ability.CPCP has excellent EMI shielding performance, which can meet the need of TMMs with EMI shielding performance.Compared with same thickness PC film, sandwich CPC film can prevent leakage phenomenon efficiently. [ABSTRACT FROM AUTHOR]

For the better operation of future electronic devices in complex situations, higher requirements of mechanical performance, especially bearing capacity, were put forward to functional composites. Therefore, the mechanical performance enhancement of functional composites had important practical application value. In this work, we reported a short carbon fiber-graphene nanoplatelets-polydimethylsiloxane (SGP)/epoxy acrylic resin (EA resin) composites with integrated thermal conductivity, electromagnetic interference (EMI) shielding, and mechanical performances using a combination method of 3D printing and vacuum impregnation. In the SGP/EA resin composite, EA resin skeleton with different cell shapes was responsible for the bearing capacity of composite samples, while the thermal conductivity and EMI shielding performance were provided by the SGP compound. When the cell shape of skeleton was circular and the filling contents in SGP compound was 15 wt% SCF and 6 wt% GNP, the SGP/EA resin composite presented best combination properties of 323.5 kPa compressive modulus, 2.13 W/(m·K) thermal conductivity, and 45.93 dB EMI shielding performance at 12.4 GHz. This work provided a facile, low-cost, and scalable method to fabricate composite samples with integrated thermal conductivity, EMI shielding, and mechanical performances. These multifunctional composites are highly promising for applications concerning heat dissipation, EMI shielding, and load-bearing devices. [Display omitted] [ABSTRACT FROM AUTHOR]