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With the rapid advance of electronics, the light, flexible, and multifunctional composite films with high electromagnetic interference (EMI) shielding effectiveness and excellent thermal management are highly desirable for next‐generation portable and wearable electronic devices. Herein, a series of flexible and ultrathin natural rubber/MXene/carbon nanotubes (NR/MXene/CNTs) composite films with sandwich structure are constructed layer by layer through a facile vacuum‐assisted filtration method for EMI shielding and Joule heating application. The fabricated NR/MXene/CNTs‐50 composite film, with NR/MXene as inner layer and NR/CNTs as out layers, not only has high EMI shielding efficiency, but also has excellent comprehensive mechanical properties at the thickness of only 200 µm. In addition, the superior environmental durability, high electrothermal conversion efficiency, hydrophobicity, and fine performance stability after periodic cyclic bending make the film possess more value in practical application.

Developing ultimate electromagnetic interference (EMI) shielding materials that can simultaneously upgrade the quality of generated electricity and the light‐thermal‐electric conversion efficiency based on traditional thermoelectric devices is crucially desired. Herein, a series of flexible multilayered phase change films (PCFs) is developed by a simple and novel origami strategy. The PCFs are first reported to improve the light‐thermal‐electric conversion efficiency by as high as 11.3%. Simultaneously, the PCFs could significantly upgrade the generated electricity on average voltage (27.3%), average current (23.8%), and lasting power outputs by 2010 times from microwatts to milliwatts. Besides, the EMI shielding efficiency of PCFs could be tuned from 39.2 to 71.9 dB by the origami process, the wide‐range EMI shielding performance could be suitable for varying occasions. Overall, this work provides a promising solution for both the preparation of multifunctional materials, high‐efficiency solar energy harvesting and upgrading electricity generation, which shows broad application prospects in EMI shielding, energy storage, and conversion.

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