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The development of flexible composites based on the transition metal carbides/nitrides (MXenes) is gaining popularity because of MXenes’ high application potentials for electromagnetic interference (EMI) shields. Here, we prepare a new type of ultraflexible composite films composed of “trashed” MXene sediment (MS) and waterborne polyurethane using a simple, facile solution casting approach. In addition to the outstanding mechanical strength and electrical conductivity, an extremely wide-range of MS contents can be achieved for the composites, resulting in EMI shielding effectiveness (SE) that may be controlled over a wide range. The X-band EMI SE of the flexible, low-density composites containing 70 wt % MS reaches 45.3 dB at a thickness of merely 0.51 mm. Moreover, the SE values of more than 34.5 dB in the ultrabroadband gigahertz frequency range including X-band, P-band, K-band, and R-band, are accomplished for the thin composites. Furthermore, the MS/WPU composite films show excellent electrothermal and photothermal performance, demonstrating the multifunctionalities of the MS-based EMI shields. Combined with the cost-efficient, sustainable, and scalable preparation approach, the ultraflexible, multifunctional composites from “trashed MXene” show great potentials for next-generation electronics. This work also opens a new avenue for the creation of innovative, high-performance, multifunctional flexible composites.

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