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Currently, carbon nanotubes (CNTs) paper (also called Buckypaper, BP) is highly promising for application in flexible electronic materials. However, the lack of flexibility and durability of BP greatly affects the comprehensive performance. Here, we propose a simple method for manufacturing a waterborne polyurethane (WPU) toughened carbon nanotube paper (WPU-BP) with excellent overall performance through vacuum filtration. In WPU-BP, as the content of WPU increased from 0 to 48.3%, the tensile strength increased from 8.08 to 16.25 MPa, and the elongation at break increased from 2.14 to 225.04%, while the conductivity decreased from 41.34 to 20.33 S/cm. The WPU-BP with the WPU content of 18.9% (CNP8) demonstrated the optimum strain sensing performance. The gauge factor of CNP8 can reach 8.57 with a response time of 145 ms. It can detect a wide range of body movements from large joint movements to slight breathing, and exhibits high stability, maintaining high stability even after 1000 cycles. In addition, CNP8 shows excellent Joule heating performance, it can reach 186.1 °C at 5 V, with heating and cooling times of only 16 and 18 s, respectively, as well as with good reproducibility. In a word, the as-prepared WPU-BP exhibits excellent both strain sensing performance and Joule heating effect, and holds significant potential for applications in heating devices and wearable sensors.

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